5th INTERNATIONAL CONFERENCE ON ISOTOPES

B R U S S E L S ? B E L G I U M ? 2 5 – 2 9 A P R I L 2 0 0 5

Roughly identical to first announcement With banner below: deadline for early registration extended

Abstract Book

1 5th International Conference on Isotopes

Brussels, Belgium, 25 – 29 April 2005 Plenary lectures

1 Nuclear geophysiology: 'radio-medicine' for planet earth T.E. Payne, A. Henderson-Sellers, D. Cohen, D. Fink, G. Jacobsen, P. Holden, S. Hollins, A. Williams ANSTO, Environment, Menai, NSW, Australia James Lovelock's seminal Gaia theory proposes that natural processes are complex and interactive at all scales leading to an Earth system which behaves as if it were a living organism. In this lecture aspects of this theory are explored in the context of nuclear research. The analogy is with nuclear medicine in which radio-tracers, radio-labels and high precision measurement techniques are applied to diagnostic and therapeutic aspects of patient care. The application of this approach to "Planet Earth" leads to the creation of the new science of "Nuclear Geophysiology". Natural variability and human impacts are leading to the perturbation of a number of components of the Earth system and the long term well-being of the planet will ultimately depend on timely remedial action based on fundamental knowledge. Major contributions to diagnostic aspects of the problem are being made by isotope techniques coupled with recent advances in environmental modelling, state of the art visualisation and a renaissance in regional and international collaboration facilitated by modern communication. These advances will be reviewed with special reference to the application of nuclear science to the fields of climate change modeling, water resource evaluation and modeling contaminant behaviour in the environment. 2 Role of alpha sources in cancer therapy B. Allen Centre for Experimental Radiation Oncology, St. George Hospital Cancer Care Centre, Kogarah, Australia The role of alpha therapy in the treatment of cancer has been a long time in incubation. Basic radiobiological studies clearly show the potential advantage of alpha over betas in terms of controlling leukaemia and micrometastatic cancer. This was not the case for developed tumours, but this situation may change in the near future. There are a number of alpha sources available, either short-lived sources from direct production via accelerators, or long-lived generators derived from isotope separation or accelerator production. However, the development of the 225Ac:213Bi generator has proven to provide a practical and efficient means of delivering targeted alpha radiation for preclinical and clinical trial applications. The development of targeted alpha therapy (TAT) for many cancers will be reviewed, key targeting vectors identified and projections made for the future application of TAT in cancer therapy. 3 PET and PET/CET are the fastest growing imaging modalities worldwide M.C. Lee Department of Nuclear Medicine, Seoul National University Hospital, Seoul, Korea Currently more than 1150 PET Centers were in operation in 2003 in the world. According to the world data of PET procedures, the number of PET studies were 255,000, 450,000, 1,300,000 and 2,500,000 in the year of 2001, 2002, 2003 and 2004, respectively. In December of 2002, National Coverage decided to expand Medicare reimbursement to include for the determination of revascularization in heart disease and epilepsy identification, as well as for 6 different types of cancer, including colorectal cancer, lymphoma, melanoma, head and neck cancer and esophageal cancer. In April, 2003, they included thyroid cancer and the use of N-13-ammonia. PET application was also approved for the reimbursement in the patients with Alzheimer's disease in September, 2004. Moreover, PET coverage decision by next request will be expected for diseases affecting women, such as breast cancer, ovarian cancer, uterine

cancer and vaginal cancer, as well as for diseases such as prostate cancer in men. The efficiency of FDG-PET was already studied in several thousand patients with malignant tumors and was found to be well documented in the international high-quality peer-reviewed literature. There are clear-cut clinical indications for FDG-PET in diagnosis, staging and therapy control, and the technique can help to improve the management of many patients with cancer. An estimated 25-30% was changed in management effect for staging and an estimated 40% was changed in management effect for recurrence in cancer, indicating cost effectiveness of PET as a direct impact. The comprehensive analysis about how many PET procedures and machines will be required in future reported 1-2 PET Centers per million inhabitants and 2000 to 4000 PET studies/million population per year will be demanded soon. PET/CT accounts for more than 65% of all current PET sales, and its share is anticipated to grow to more than 95% over the next years. Korea had a really great success for the promotion of PET technology. Currently 43 positron emission tomography (PET) machines are being operated (12 PET and 31 PET/CT) in 35 PET Centers throughout the nation. The molecular information available through PET enables clinicians to identify the functional content of anatomic abnormalities and to categorize them as malignant or benign. PET/CT offers remarkable advantages. These include shorter image acquisition times resulting in greater patient throughput and thus more efficient instrument utilization; improved lesion localization and identification; and more accurate tumor staging. 4 Diagnosis and cure: radioisotope applications in the offshore oil and gas industry J.S. Charlton Company Scientist, Tracerco. For well over half a century investigative techniques based upon radioisotope technology have been applied to trouble-shooting and process optimisation in the oil and gas industry. These categories of application are referred to generically as "process diagnostics" The continuing development of offshore oil and gas reserves has involved a high degree of technological and engineering innovation. To meet the new challenges posed by offshore operations, the radioisotope technology used for process diagnosis has also been continuously adopted and modified. Through case studies, this paper illustrates some important ways in which radioisotopes are currently used to diagnose the cause of problems, both sub-sea and on the production platforms. Sub-sea, sealed sources of radiation and radioactive tracers are used routinely to confirm the integrity of production platforms and to trouble shoot pipeline problems. On the platforms, the main areas of application are the investigation of performance problems in gas dehydration equipment and production separators. To complement the diagnostic use of radioisotopes, nucleonic instruments have been developed to monitor and control offshore production processes. In this sense, radioisotope technology provides not only accurate diagnoses of problems, but also the means to cure them. This is exemplified by reference to a novel nucleonic instrument, which has been developed to help optimise the performance of 3-phase production separators, a notoriously difficult control application. The growing usage of radioisotope technology offshore is testament to the enormous economic benefits derived, by the oil and gas industry, from its applications. The paper presents examples of some of the benefits that have been achieved.

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5 Multi-interdisciplinary approach in the palaeoenvironmental reconstruction study in Brazil L.C.R. Pessenda1, M.P. Ledru2, S.E.M. Gouveia1, R. Aravena3, A.S. Ribeiro4, A. Sifeddine5, J.A. Bendassolli6 1Centre for Nuclear Energy in Agriculture, C-14 Laboratory, Piracicaba, Sao Paulo, Brasil 2IRD, Botanic, Montpelier, France 3University of Waterloo, Earth Sciences, Waterloo, Canada 4University of Sergipe, Biology, Aracaju, Brazil 5IRD, Geochemistry, Bondy, France 6Universityo f Sao Paulo, Stable Isotope Laboratory, Piraciacaba, Brasil In palaeoenvironmental reconstructions the results inferred from lacustrine sediment pollen analysis and carbon isotopes from soil organic matter (SOM) records have rarely been compared in a same area for the same time interval. In this paper we present the first results of this multi/interdisciplinary study. The study site is located in the Barreirinhas region, Maranhão State, NE Brazil. Soils were sampled for d13C analysis and buried charcoal fragments in the soils were radiocarbon dated. Three soil profiles collected in forested areas around the lake (Lagoa do Caçó) and five in a forest - woody savanna (mixture of non arboreal and arboreal species) ecotone located approximately 10 km southeastern of the lake were studied. A high resolution pollen record was obtained from lake sediments, showing forest vegetation was predominant in the area in the early Holocene. From approximately 10,000 14C yr BP the pollen spectrum gradually changed, suggesting the dominance of open savanna communities, that were transformed to a more forested landscape (woody savanna) from approximately 7500 yr BP. The lake sediments also record fire signals (charcoal particles) during the Holocene. The presence of buried charcoal fragments at several soil depths also suggested the occurrence of palaeofires during the Holocene. The d13C analysis SOM indicates that from between approximately 10,000 yr BP and 9000 yr BP to ~4000 yr BP, a woody savanna prevailed at two sites around the lake, probably reflecting a drier climate. From ~4000-3000 yr BP to the present, the results indicate a moderate and progressive increase in the arboreal vegetation around the lake, due to the return to more humid climate conditions probably similar to the present day. The carbon isotope results indicate the presence of an open vegetation since the early Holocene at the site located 10 km from the lake. In general, there is agreement between the palaeovegetation pattern inferred from the pollen and carbon isotopes data. However, a much less uniform landscape, with a mosaic of different ecosystems at any given time is inferred from the carbon isotope record. 6 Research with light-ion cyclotrons in Europe H. Stamm, K. Abbas, N. Gibson, U. Holzwarth Institute for Health and Consumer Protection, Biomedical Materials and Systems Unit, Ispra, Varese, Italy At present about 300 to 400 cyclotron exist worldwide, of which 100 to 150 are located in the countries of the European Union. Most of them are dedicated to routine medical isotope production in hospitals. Only a few versatile light ion research cyclotrons (approximately 20 to 30) with particle energies greater than 20 MeV and various particle types are still in use. In addition there are some heavy ion machines mostly used for studies in nuclear physics. Frequently, activities at such cyclotrons are at risk because of the high costs involved, and many of the facilities have been closed in the recent years. This deserves a closer look at the societal benefits of such infrastructures and the need to maintain them. Light ion research cyclotrons are very flexible machines and are used in different areas ranging from basic research in nuclear physics to biomedical applications, trace element and material studies including industrial applications. Their strength lies in their versatility in particle energy, particle type and beam current which makes them suitable for research and industrial applications. Such research cyclotrons are very unevenly distributed around Europe, with the greatest concentration (approximately 10) being in Belgium, Holland and the Western region of Germany. The other facilities are widely scattered in various other member states. As a

whole, this forms a most valuable infrastructure in Europe. Application driven projects performed with light ion cyclotrons have a wide importance and provide direct benefits to the European citizen and industry. The use of these research facilities tends to be primarily in-house, or by research groups from nearby universities and research centres. This leads both to a very fragmented and un-coordinated approach to development of cyclotron-related technology and applications. Moreover, in the era of molecular medicine and the possibility of new molecular therapies, there may be severe shortfalls in the production capacity of cyclotrons to provide sufficient quantities of radioisotopes for new diagnostic and therapeutic agents across the EU. This paper will illustrate and review important activities using light ion cyclotrons demonstrating the application oriented need. It will underline the necessity of better coordination of research endeavours to achieve a better utilisation of such facilities and creation of a greater visibility underlining the relevance of the activities for all citizens. 7 The role of isotope separation techniques in future medical isotope production programs H.L. Ravn

CERN, PH Department

In conjunction with the GeV proton beams of MW power planned for a number of new major physics-research facilities an opportunity for production of new radioisotopes for future medical use in a fully parasitic mode is described. Recent new developments in systemic radionuclide therapy now strongly call for radioisotope preparations with new characteristics that have not been available before. Especially important for the new applications is high specific activity of the radiotracer in therapeutic amounts. Conventional methods in medical isotope production have reached their technical limitations and the progress is limited by the availability of radionuclides with the wanted characteristics. These are either only or best produced in high-energy spallation and fragmentation reactions. The target and ion-source techniques developed for making the high purity radioactive ion-beams (RIB) at CERN ISOLDE is now a well-documented new type of rapid, efficient, continuous and automatic radiochemical separations. Its electromagnetic Isotope Separator On Line (ISOL) allows producing efficiently very pure samples of almost all radioactive isotopes with the highest possible specific activity, i.e. the carrier free form. Until now these techniques have exclusively been used to make RIB of short-lived species for scientific purposes. It is now generally recognized that simplified variants of these techniques also will allow harvesting samples of longer-lived, high purity and carrier free radio nuclides as a byproduct from the spent target material and spent beam absorbers. A typical example of the “heart”

of such a facility is shown in the figure. In particular it has produced “exotic” radioisotopes that hitherto were not available on

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the market for medical use but only in amounts that has allowed the R&D work and validation of the methods. We believe that the time has come to prepare for more rational and large-scale industrial radioisotope production methods using the ISOL target techniques. The production sites should be put in synergy with one of the MW targets planned future physics projects like EURISOL where the radioactivity production may be up to 5 orders of magnitude higher than at present facilities. 8 Opportunities in European Molecular Medicine: a nuclear medicine’s perspective B. Brans, W. Oyen European Association of Nuclear Medicine, Vienna, Austria In the last decade, molecular medicine is a progressively growing discipline. As fundamental insight in the molecular processes involved in pathophysiology increased and the improvement of technology resulted in new and better devices and in new specific compounds, it is now considered an extraordinary opportunity for research investment. It has both diagnostic as well as therapeutic branches, and has its roots in both molecular biology and cell biology. Molecular imaging consists of magnetic resonance imaging (MRI), in-vivo optical imaging and nuclear medicine techniques. From a nuclear medicine's perspective positron-emission tomography (PET), gamma camera imaging (SPECT) and autoradiography are available for basic and human research. In this presentation, multiple examples are given to highlight the extra-ordinary potential of radionuclide-based molecular imaging. These modalities allow highly sensitive whole body monitoring for disease such as cancer metastases. Combined with computerized tomography (CT) into one machine, the so-called PET/CT allows a "one-stop-shop" oncology staging examination of the future for many tumours. Molecular imaging fulfils modern oncology's view on biological characterization of neoplasms (e.g. differentiation, invasiveness, metastatic potential, proliferation, hypoxia, receptor status) in order to develop and monitor therapies. Molecular targets defined by molecular medicine can be effectively studied by imaging and biodistribution studies of radiolabeled compounds, facilitating and accelerating the search for effective anticancer treatments. Similar potential is present in other fields of medicine, such as cardiovascular and neurological diseases, infection/inflame-mation. When a compound is labelled with "therapeutic" isotopes (β-emitters and perhaps in the future α-emitters), it can be used to deliver specific targeted radiotherapy, sometimes referred to as "molecular radiotherapy". This approach results in cell death by itself, but can also be combined with cytotoxic of cytostatic drugs to enhance the effectiveness in a synergistic way. These new paradigms are unique in combining diagnostic imaging, radiation therapy and nuclear medicine by implementing basic biological knowledge, and will stimulate new collaborative research, training and education. 9 Production of radioisotopes for nuclear medicine: tomorrow neds for reactor availability in Europe H. Bonet, B. David National Institute for Radioelements (IRE) , Fleurus, Belgium Today, production of reactor radioisotopes for use in Nuclear Medicine is based in Europe on irradiation of targets in a network of multipurpose test reactors including mainly HFR (Nl), BR2 (B), OSIRIS (F), FRJ-2 (D), STUDSVIK (S), MARIA (PL)... Besides the fact that these reactors are aging and that in the rest of the world, the availability of new reactors with appropriate performances and of large production facilities is still questionable, recent decisions to shutdown FRJ-2 and STUDSVIK reactors raised again the issue of reactor availability in Europe for tomorrow. It is the right time for investigating the needs for investments securing enough capacity of irradiation for responding to very demanding requirements for ensuring the security of supply of key isotopes for the Nuclear Medicine Community.

Based on IRE's experience as a major producer of fission radioisotopes (Mo99, I131, Xe133), irradiating HEU targets in a network of 4 reactors, we analyzed the needs and defined the technical and economical requirements associated with the renewal of the reactor network optimal for radioisotope production. This paper will review the following key factors and possible options: - very high availability and reliability, easy maintenance, high safety margins and low environmental impact; - a large number of target irradiation facilities, with high thermal neutron flux, high cooling capacity, easy handling of targets during operation; - low investment and operating costs (including fuel cycle) justifying the economy for producing less than 50% of the radioisotope world demand. For securing the necessary back-up production, at a first stage a renewed network of multipurpose reactors should keep available sufficient irradiation facilities and in further time alternative options such as a second dedicated reactor or an ADS (Acceraltor Driven System) might be included in the back-up reactor network. For ensuring the security of supply by addressing common mode risks, the back-up network should warranty sufficient redundancy and diversity characteristics with regard to design, location, operating organization... It should ideally propose upgraded performance (eg. higher thermal neutron flux) for more specific isotopes production (eg. Ir192, W188,. ..). Today, it is time for all partners involved directly or indirectly at different stages of the supply of radioisotopes and in particular the different authorities, to work together for addressing the threat of shortage of supply of key radioisotopes needed by Nuclear Medicine in Europe and in the World.

5ICI 4 Oral Presentations

Track 1 - Session 1: Isotope Programs 10 Support to development of technology and national capability for production and utilisation of radioisotope products. IAEA's facilitator role N. Ramamoorthy, M. Haji-Saeid IAEA, Vienna, Austria Radioisotope products in use in diverse fields are available from industrial companies. In view of half-life logistics and cost effectiveness, indigenous production capability is sought by developing countries. International Atomic Energy Agency has been fostering capacity building measures in Member States (MS) by two strategies, Coordinated Research Projects (CRP) and Technical Cooperation (TC) Projects. Research Reactors and charged particle accelerators (medical cyclotrons) are used to produce useful quantities of radioisotopes in MS. Import of bulk radiochemicals for preparation of finished products is also known , especially using fission produced Mo-99 for Tc-99m generators and Ir-192 for radiography sources. Excellent progress is notable in MS, some labs even functioning on commercial basis, for effectively catering to local and regional markets, e.g. in Argentina, Brazil, Chile, Hungary, Indonesia, Iran, Poland, Thailand, Turkey, Uruguay, Vietnam, to cite a few. CRPs are thematic pursuits over 3-5 years involving 10-15 groups, from both developed and developing countries. Three types of projects can be cited, Adaptive Research, Applied Research and Strategic Research. Harmonised procedures for production, quality control testing and applications have emerged in many instances apart from creation of expertise in R&D pursuits in MS. Some CRPs in the area of radioisotope production are: Standardized high current solid targets for cyclotron production of diagnostic and therapeutic radionuclides; Development of reference charged particle cross-section database for medical radioisotope production; Optimisation of production and QC of radiotherapeutic radionuclides and radiophar-maceuticals; Development of radioactive sources for emerging therapeutic and industrial applications; Development of generator technologies for therapeutic radionuclides and Nuclear data for production of therapeutic radionuclides. Transfer of relevant technology to interested MS is achieved through TC Projects. Successful implementation in recipient MS has led to regular indigenous production and utilisation of many radioisotope products. Important examples of success stories of fostering indigenous radioisotope products are, (a) Production of Tc99m generators and kits in Indonesia, Iran, Kazhakstan, Pakistan, Syria etc. and (b) Medical cyclotron production of SPECT and PET tracers in Brazil, Czech Republic, Iran, Korea, Syria etc. 11 Progress report for the production of medical radioisotopes at Korea Institute of Radiological and Medical Sciences J. Kim, D.H. Lee, G.I. Ahn, J.S. Lee, H. Park, C.W. Choi, K.S. Chun KIRAMS, Cyclotron Application, Seoul, Korea With the facilities of the High Current Proton Cyclotron (IBA), radiochemistry laboratory and Good Manufacturing Practices, the interesting radionuclides of positron emitters for PET images and gamma ray emitters for SPECT are produced via various (p,xn) reactions. Several different targets have been developed to enhance the production yield for specific radionuclides: gas targets employed for C-11, F-18 and I-123 radionuclides (Nordion), a liquid target used only for the F-18 nuclide, and solid targets (IBA) prepared for the production of Ga-67 and Tl-201 nuclides. A Cyclone30 cyclotron (IBA) installed at 2002 and has four external beam lines with the target station for a specific radionuclide production. One external beam line is expanding by increasing the number of designed target chambers for the R&D purpose and for the backup in order to maintain the uninterrupted production in case of target chamber malfunction or foil breakdown. A water target with a grid window and a gas target are designed and constructed at KIRAMS. Radionuclidic impurities are determined by the gamma-spectrometer with a high purity Germanium (HPGe) detector. The theoretical yields based on recommended database are calculated

and compared with these yields. The comparison of activities and impurity level deduced at energy ranges and target conditions will give significant help to target preparation and optimization of the radioisotope production. The production of five radionuclides (C-11, F-18, I-123, Ga-67, Tl-203) is carried at KIRAMS with enriched target materials. The average yields of F-18, I-123, G-67, and Tl-201 radionuclides are 90mCi/uAh, 10mCi/uAh, 3mCi/uAh, and 1mCi/uAh at the end of beam (EOB), respectively. The radiochemical purity of product has been achieved higher than 99.7% and the production yield closely depends on target thickness, bombarding time, and growing time. The enriched target materials of Zn and Tl are coated on Cu-plate by an electro-deposition method and the irradiated target with 220uA proton beam is then transported into dedicated hot-cells of the separation module developed by KIRAMS. The enriched target materials can be recycled for the next irradiation after proper chemical treatments. 12 Status and prospects of radioisotope technology in China J. Zhang China Institute of Atomic Energy, Beijing, China The paper does the retrospects to the developing history of China's radioisotope technology which initiated in 1958 and formed its own radioisotope subjects and radioisotope industries gradually during the past 46 years. With the first heavy water reactor (HWR) and first cyclotron coming to running in 1958 as the starting point, the development of China's radioisotope technology underwent about four periods. They were the initiating period of R & D and applications (1950s to 1970s), the developing period with industrial applications as the focal point (1980s), the developing period with medical applications as the focal point (1990s) and the developing period of the standardization and market competition of isotopic enterprises (began from year 2000). During these periods, radioisotope technology did great contributions to the development of Chian's national medicine, industry and agriculture and so on. For the current status of China's radioisotope technology, the description on the radioisotope production and applications in the fields of medicine and industry was given. China now has 5 reactors, 2 sets of 30 MeV advanced cyclotrons and 40 sets of PET center used small cyclotrons for radioisotope production. Except large amount of 99Mo and 60Co, fission produced nuclides and transuranic elements for radiation sources preparation are still relied on importing, China could produce and offer most of the routine used isotopes for domestic needs, e.g. for medical uses it provides diagnostic and therapeutic radiopharmaceuticals for 500 sets of SPECT, 50 sets of PET, 800 hospital's nuclear medicine departments and more than three thousands hospital's RIA kit users; for industrial applications, about thousands sets of isotopic instruments and nuclear control system were equipped in many fields for various measurements and detections, and the radioactive sources, labeled compounds and tracers are acting as the powerful role for supporting the development of radiation applications, energy resources and life sciences. The radioisotope technology has won considerable economical and social benefits, and a complete developing system of radioisotope production and application industry has formed in China. The anther finally describes the prospects of the application of radioisotope technology in the future industrial modernization, rising industry development. 13 Production of medical radioisotopes in NRCAM using Cyclone30 G. Raisali Atomic Energy Organization of Iran, Nuclear Research Center for Agriculture and Medicine, Karaj, Iran At present more than 90 private and governmental nuclear medicine centers are giving services to the patients in Tehran and other major cities in Iran. About half of these centers use cyclotron-based radiopharmaceuticals from Nuclear Research Center for Agriculture and Medicine (NRCAM) in addition to the reactor products. Production of cyclotron-based radio isotopes has begun in Iran (in NRCAM) since 1994. The production facility is located in Karaj about 40 km from Tehran. The main facilities are cyclone30

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cyclotron from IBA, target preparation laboratory and workshop, hot laboratories, QC laboratories, and a dual head gamma camera system with coincidence capability suitable for SPECT and PET imaging quality assessment of the products. An electro-magnetic isotope separator is also operational in the center for production of some isotopic enriched target materials such as Zn-68. The main medical radioisotopes and radiopharmaceuticals produced in NRCAM are: 1500 mCi of Tl-201 in chloride form per month, 300 mCi of Ga-67 citrate per month, Rb-Kr-81m generators, and In-111. FDG and I-123 have been also produced in research scale. The research phase for the production of Co-57 and Pd-103 isotopes have been also completed, and the encapsulation of these isotopes as standard calibration source and brachytherapy seeds is under development. Now, NRCAM has focused on the implementation of the GMP and QA requirements for higher performance of the system and higher quality of its products. In this paper some details concerning cyclotron-based radioisotopes and radiopharmaceuticals production in Iran will be presented. 14 Production and development of radiation sealed sources H. Han1, K.J. Son1, U.J. Park1, J.S. Lee1, K.B. Park2 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Daejeon, Korea 2Korea Atomic Energy Research Institute, Center for HANARO Applications Research, Daejeon, Korea The Korea Atomic Energy Research Institute (KAERI) has utilized the High-flux Advanced Neutron Application Reactor (HANARO) since 1995 and the radioisotope production facilities (RIPF) since 1997 for the production of radioisotopes. Specially, a variety of sealed radiation sources for industrial and medical applications has been developed or under the development at KAERI. The basic technologies and fabrication equipment such as a laser welder, a TIG welder, viewing system, and automatic welding devices for the production of these sources have been developed and installed. For the quality control of the products, ISO 9002 quality assurance system has been established and applied for the entire production processes of the sealed radiation source. Currently, 192Ir sources for NDT and brachytherapy, and 60Co source for gauge, are developed and commercially supplied to users. In 2003, KAERI supplied 83 kilocuries of such sealed sources to domestic users. Upon successfully commercializing high specific radiation sources, KAERI extends its research area to the development of micro-sources. On behalf of this effort, current research activities focus on the fabrication of 125I seeds and 169Yb and 75Se as low energy gamma cources. Preliminary studies with a ceramic rod, which is treated with silver nitrate show that it can be used as a good iodine carrier for the 125I seeds. In addition, various acceptable welding schemes have been examined to find the best sealing technique. To produce 169Yb sealed sources, compacting and sintering of yttrium have been studied. This seal source capsule consists of a pure aluminum inner capsule, in which yttrium pellets are, and a titanium outer capsule. A neutron irradiation experiments have been performed to the encapsulated yttrium which is in form of 1mm x 1mm pellet by using HANARO. 15 The management, control and monitoring of the radioisotope production lifecycle through web-based applications A. Dana, R.H. Prinsloo, G. Ball NECSA, NTP, Pretoria, South Africa NTP Radioisotopes (Pty) Ltd produces nuclear technology based products that are used primarily in health and industrial sectors across the globe. We are constantly developing applications that will drive safety, efficiency and quality standards throughout our organisation. These systems facilitate production planning, assists in processing orders, use computational algorithms to perform calculations and provide accurate and timely information to decision-makers both on the ground and at management level. It ensures data integrity is kept at all levels by eradicating duplication and reduces human error inherent in manual methods Based on the speed and volume of information gathered we now know much

more about customer behaviour, which means that we can provide a better service through the analysis of extracted data. Some of these applications include Irradiation Management, Isotope Orders and Dispensing, and Container Tracking systems. The Irradiation Management system forms an integral part of the isotope lifecycle. Irradiation of samples within the SAFARI-1 research reactor are scheduled, planned, tracked and monitored from multiple access points throughout the plant, using this web based application. Elements such as electronic access control, automated quality checkpoints, decisions support and report generation streamlines production and maximizes reactor utilization. The dispensing of products is of critical importance to us and our clients. To improve the safety, efficiency and quality of the dispensing of radioisotopes, an in-house web-based application was developed. The system controls and monitors the ordering, production planning, flight booking and dispensing of an isotope to a particular client. The Container Tracking System tracks the entire lifecycle of our type B(U) containers. This includes storing information about their history, from inception through to orders, maintenance, quality, and eventual decommissioning. Together, these interrelated web-based applications support an environment for safer and more efficient isotope production, synergising the needs of the client, the knowledge of the engineer and the skill of the operator. Track 1 – Session 2: Isotope Production Technology 16 The influence of a nuclear prehistory on transport rate of impurity "hot" atoms of 67Ga in the irradiated metal zinc I.E. Alekseev1, V.V. Lazarev2, S.R. Tkharkakhova1 1State University, Radiochemistry, St. Petersburg, Russia 2State University, Nuclear Physics, St. Petersburg, Russia In previous publications (see for example [1]) it was shown, that the velocity of migration of radioactive microimpurities (formed as a result of a nuclear change) in irradiated metals is instituted by a nuclear prehistory. In the present work this problem was explored in detail. In selected system "zinc - impurity atoms of 67Ga" it is possible to gain the same impurity "hot" atoms via different "nuclear channels" and to explore their behavior depending on a nuclear prehistory. The carried out experiments have shown, that the basic tendency in diffusion behavior of impurity "hot" atoms are clearly traced - direct dependence of transport rates of 67Ga from a degree of radiation damage of zinc targets at bombardment. The velocity of migration of impurity atoms is instituted by "unsoundness" of structure after bombardment and depends on the type (p, d or 4He), intensity of beams of charged particles and total fluence. [1] I.E. Alekseev, A.E. Antropov General trends of diffusion, physical and chemical behavior of transmutation radionuclides during thermal annealing of irradiated metals // Radioactivity & Radiochemistry, Vol. 11, 2, pp. 38-43. 17 Theoretical evaluation on Sr-89 recovery fromt he gas phase in the argus Y.J. Shin, H.S. Shin, I.S. Kim, S.H. Cho, S.Y. Oh, K.B. Park Korea Atomic Energy Research Institute, Daejeon, South Korea Sr-89 has been used for pain palliation instead of drugs when treating cancer. There are two conventional Sr-89 production methods, such as Sr-88(n, γ)Sr-89 and Y-89(n, p)Sr-89. However these methods have an extremely low productivity due to the small cross-section and demand highly enriched and purified isotopic targets to be irradiated. On the other hand, a more efficient method for the production of Sr-89 has been introduced conceptually by Russian scientists. The new technology based on a solution nuclear reactor(ARGUS) with aqueous uranyl sulfate fuel is entirely different from the conventional methods. Sr-89 in the ARGUS can be produced as a result of the decay chain like Se-89→Br-89→Kr-89→Rb-89→Sr-89. The decay chain informs us the possibility to recover Sr-89 from the gas phase during the Kr-89 existence. The difference of half-life between Kr-89 and Kr-90 offers a chance for the isotopic separation of the strontium. In the US Patent 6,456,680,

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the conceptual process to recover Sr-89 consisted of the solution nuclear reactor, the primary decay tank to remove Sr-90, the secondary decay tank to precipitate Sr-89, and the circulation gas pump. Based on the mechanism of the Sr-89 formation and the introduced process, the dynamic tanks-in-series model has been adopted to analyze theoretically the Sr-89 productivity. The effects of the gas flowrate and the volume of the decay tank on the Sr-89 recovery were also evaluated in this study. The optimized operating condition has been finally proposed. As a result of the study, the maximum productivity of Sr-89 is about 1 Ci/kWt/year in the ARGUS facilities with key parameters of 250 operation days and 6,000 campaigns per year. 18 Developing a method for the production of high specific activity 117mSn from tin oxides using the Szilard-Chalmers effect D. Jansen1, J.R. Zeevaart2, Z.I. Kolar3, G.C. Krijger3 1Necsa, Radiochemistry, Brits, North West, South Africa 2Necsa, Radiochemistry, Pretoria, South Africa 3Department of radiation, radionuclides and reactors, Faculty of Applied Sciences, Delft University of Technology, The Netherlands In the research and development of potential radiopharmaceuticals part of the challenge is the production of the radionuclide with high enough specific activity (i.e. high amount of radioactivity per mg of metal) and radionuclidic purity. In our consideration for identifying effective therapeutic agents for the palliation and treatment of bone cancer metastasis 117mSn is ideal. This is due to the chemical properties of Sn and the radiation properties of this isotope (half-life 13.6 days, discrete range of 0.2 - 0.3 mm). The proposed technique to obtain high specific activities of Sn-117m is based on the Szilard-Chalmers effect. The principle behind the technique is the capture of the desired recoil activity (Sn-117m) in a chemical form that differs from the original neutron irradiated target material. For our investigations we considered irradiating SnO and SnO2 suspended in aqueous solutions. The desired activation product (117mSn) is ejected from the insoluble tin-oxide crystal matrix during irradiation, upon which these active tin-ions are taken into solution - the surrounding medium - from whence they are later extracted. Experiments were conducted to optimize parameters such as maximum liquid content and pH of the solution. It was important to ensure that the tin-oxide remained submersed in the recoil capture medium for the entire duration of the procedure - especially during irradiation. The pH was lowered so as to avoid precipitation of the 117mSn due to hydrolysis - which would have made it difficult to separate from the inactive oxide. 19 Sol-gel processed ceramics for 99Mo/99mTc generator materials J.S. Lee1, H.S. Choi1, O. Choi1, U.J. Park1, K.B. Park2, H.S. Han2 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Yuseong-Gu, Daejeon, Korea 2Korea Atomic Energy Research Institute, Center for HANARO Applications Research, Yuseong-Gu, Daejeon, Korea Sol-gel processing has been employed for more than 20 years to develop pure ceramics, composite metal oxides, and organo-ceramic hybrids in the applied material sciences. This processing method has mild reaction conditions that make it possible to produce such materials with various material properties. In this study, a sol-gel processing scheme is adopted to develop a silica and an alumina with zirconium chloride functionality. Physico-chemical properties of the developed materials are characterized as well as the measurements of molybdenum uptake capacities. The developed material has a high enough molybdenum uptake capacity (>200 mg/g) to produce 99Mo/99mTc generators with neutron-irradiated enriched molybdenum-98. Demonstration studies have been undertaken for the loading efficiency of the molybdenum and the technetium elution in a column. The loading and elution studies are performed by using a 0.8cm ID chromatography column filled with the synthesized adsorbents and alumina backup layers. Experimental results show that the elution efficiency of the column ranges from 85 and 90% of the expected values.

20 Enrichment of the Yb-176 stable isotope for the production of the therapeutic radioisotope Lu-177 H. Park, D.H. kwon, Y.H. Cha, S.M. Nam, S.K. Kim, J.M. Han, Y. Rhee, D.Y. Jeong, C.J. Kim Korea Atomic Energy Research Institute, Laboratory for Quantum Optics, Daejeon, Korea Lu-177 is known as a promising therapeutic radioisotope for the curative treatment of cancer using the labeled protein. A no-carrier-added (nca) Lu-177 can be produced by a neutron capture reaction of isotopically enriched Yb-176 in a nuclear reactor. For this application, Yb-176 should be enriched to more than 95% from the natural abundance of 12.73%. With this background, we developed laser enrichment technology of a Yb-176 isotope. Our system consists of laser system, Yb vapor generating system, and photoionized particle extraction system. For the laser system, we developed a diode-pumped solid-state laser of high-repetition rate and 3-color dye lasers. Yb vapor was generated by heating solid Yb sample resistively. The photo-ion produced by resonance ionization were extracted by a devised extractor. As a result, we succeeded to produce the enriched Yb-176 with the abundance more than 95% in the form of Yb(NO3)3. 21 Highly-enriched stable isotopes - starting material for the heavy-ion beam at GSI B. Lommel, W. Hartmann, R. Hollinger, A. Huebner, B. Kindler, J. Steiner, K. Tinschert Gesellschaft für Schwerionenforschung, Darmstadt, Germany At GSI heavy-ion beams up to 2000 MeV/u are available for basic and applied research in atomic physics, biophysics, material research, nuclear physics and plasma physics. Depending on the requirements of the experiment, the ion source has to be fed with enriched isotopic material and the targets have to be made out of enriched isotopic material. Depending on the type of the ion source, medium or high-enriched isotopic material is needed. Frequently the material is not easily available in the wanted chemical or physical form. The resultant problems for the application in the source are going to be discussed exemplarily. Track 1 – Session 4: Isotope Production Reactor based 22 The production of Cu-67 as pharmacokinetic and toxicokinetic copper tracer via the Zn-67(n,p) reaction J. Hattink1, B. Ponsard2, A.V. Harms3, G. De Boeck1, G.C. Krijger4, R. Blust1 1University of Antwerp, Biology, EB§T-laboratory, Antwerpen, Belgium 2SCK-CEN, Radioisotopes & ASC Silicon, Mol, Belgium 3National Physical Laboratory (NPL), Centre for ionising radiation metrology, London, United Kingdom 4Reactor Institute Delft, Radiation and Isotopes for Health, Delft, The Netherlands 67Cu has many ideal properties for pharmacokinetic and toxicokinetic research. It has a half-life of 2.58 d and decays to stable 67Zn. It is a β--emitter with maximum energies of 392 keV (57%), 484 keV (22%), and 577 keV (20%). Its γ-energies of 91 keV (7%), 93 keV (16%), and 185 keV (49%) allows repetitive live counting of individual subjects over a reasonable period. The carrier free specific activity is 2x1018 Bq/mol, reachable via the 67Zn(n,p) reaction. Here we report this 67Cu production and its radiochemical purity. The 67Cu-tracer was used in fish physiological research. We produced 67Cu by irradiation an enriched 67Zn target in a fission neutron field of 3x1014 n/cm2/s in the core of the BR2-reactor (SCK.CEN, Mol, Belgium) for 21 d. After irradiation, mainly 67Cu (460 MBq) and 65Zn (375 MBq) were formed, although also smaller quantities of other radionuclides (60Co, 114mIn, and 125Sb) were detected. Purification of 67Cu was performed using conditioned

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anion exchange columns. First, most of 65Zn was extracted by using 8 M HCl. Subsequently, copper was reduced with ascorbic acid and the Cu(I)chloride-complexes separated from remaining impurities in 2 M HCl. 67Cu was extracted by re-oxidising with 4% H2O2 in 2 M HCl. The purified product had a half-life of 2.576 ± 0.004 d and showed a 67Cu recovery of 86 ± 2 %. Contaminants were adequately removed, only 0.002% of the initial 65Zn and minute amounts (in the order of kBq) of 60Co and 114mIn were present. The actual 67Cu specific activity was 1x1x Bq/mol, since trace amounts of stable copper was present in the zinc target (0.01%). The crossection for thexZn(n,p) reaction determined from this irradiation was 0.77 mb, corresponding with the 0.77 ± 0.09 mb reported by O'Brian (1969) determined under similar conditions. However, it is threefold higher than the reported crossection of 0.26 mb in the ACSELAM database. The presence of trace amounts of other nuclides, in particular 114mIn, can disturb the 67Cu-signal, despite the high 67Cu to contaminant activity concentration (>15000), due to possible bioconcentration of any of the impurities. This was not the case in three freshwater fish species, an euryhaliene fish and oligochaete, if any uptake of these contaminants occurred at all. With the present material and purification methods applied, the forming of impurities can be decreased by purification of the target prior to irradiation. A 20-fold increase in the 67Cu specific activity can than be achieved. 23 Transport fuel cycle in the production of Fission Mo-99 F. De Smedt1, P. Bizet2, B. David3 1TRANSRAD, Belgium 2NCT, France 3National Institute for Radioelements, IRE, Belgium Mo-99 has become over the years probably the most important radio isotope in the Nuclear Medicine.Mo-99 is a fission product of irradiated HEU.This irradiation takes place in research reactors, that can provide a sufficient high flux in neutrons. The operations of the research reactors and the safe supply of fresh HEU/LEU fuel is a need for guaranteed operations and reliable service to the Mo-99 production companies. The production of Mo-99 starts with the safe transport of non-irradiated HEU targets from France to the research reactors in France, Belgium, Germany and The Netherlands. After irradiation, the HEU targets have to be transported as soon as possible to the production facilities to minimize the loss in activity due to the limited half-life of Mo-99. After purification, the bulk Mo-99 has to be transported to the Radiopharmaceutical plants as soon as possible for the same reason of limited half-life. As the purification of Mo-99 from the irradiated HEU targets is a chemical process, the transport of the liquid waste and the recovery of the remaining HEU take special care as well. Transport licensing, package validation, physical protection, lashing of the packages whilst transport, nuclear liability insurance and quality assurance are special items linked to the logistics of this fuel cycle which need particular attention in order to comply with national and international regulations. These logistics have to be carried out by specialised companies that possess the necessary know-how in transportation and regulations, the necessary permits in the different transiting countries, the approvals of the Competent Authorities in the transiting countries, the personnel with the required safety screenings and the necessary means in order to assure physical protection of documentation and materials. All these points have to be under control before the start of a transport, which sometimes is a very critical path and makes the transports "just in time". 24 High specific activity Tin-177m reactor production at RIAR Y.G. Toporov1, O.I. Andreyev1, F.Z. Vakhetov1, V.D. Gavrilov1, S. Shrivastava2 1Federal State Unitary Enterprise "State Scientific Center of Russian Federation - Research Institute of Atomic Reactors" - Russia 2Brookhaven National Laboratory, Upton, NY, USA

Nuclear-physical and biochemical properties of tin-117m and some its compounds allows one to consider them as a prospective radiopharmaceuticals for palliation of bone metastases and treatment of some other cancers. To minimize chemical toxicity of tin preparations arising from en excess of complex agent high specific activity tin-117m should be used for synthesis of radiopharmaceuticals - more than 8 Ci/g. Under the BNL-RIAR joint research project the possibility of production of Sn-117m with required specific activity using SM high-flux reactor has been demonstrated by calculation and experimentally, parameters of radionuclide have been determined. Reaction of Sn-117m production from Sn-117 is a threshold one and takes place in fast neutrons (En>0.1 MeV). So, irradiation positions in the active core of the SM reactor with maximum fast neutron flux density (2.1015 cm-2s-1) were used for irradiation. An average cross section value of the production reaction was determined by averaging of the energy dependence of the cross-section of inelastic neutron scattering on Sn-117 nuclei using calculated neutron spectra. For cells of active core of the SM reactor that value was found to be 140 mbarn. Using this value for calculations has demonstrated that in a regular reactor campaign (18 effective days) specific activity of Sn-117m can reach 17 Ci/g at EOB. Irradiation during two campaigns allows increase of specific activity up to 23 Ci/g. Irradiation of experimental samples of tin metal enriched with tin-117 up to 92% has proved results of calculations. Technology of radiochemical processing of irradiated tin samples includes the following stages: a) dissolution in hydrochloric acid, b) ion exchange purification from impurities, c) reduction of tin to metal state by cementation, d) preparation of the final form of the product (SnCl2 or SnCl4) by metal dissolution in hydrochloric acid. Radionuclide purity of the product is not less than 99.99%. Certification of the final product is carried out by gamma-spectrometry. Specific activity of Sn-117m is determined by radiometry or mass-spectrometry. Radiopharmaceutical - 117mSn (IV)-DTPA - was synthesized and studied by BNL. It was demonstrated that parameters of high specific activity Sn-117m produced by RIAR fulfill requirements for production of compounds with decreased chemical toxicity. These compounds have had high in vitro stability (>99% after 30 days); in vivo distribution in bones studied in the mouse model has complied to the predicted one. The research was implemented jointly by RIAR and BNL with the financial support of DOE. 25 188W/188Re generators of 1 Ci activity: results of 7 month performance study R.A. Kuznetsov1, C. Daming2, A.N. Pakhomov1, S.I. Klimov1, Y. Honwei2, C. Benzhu2 1Federal State Unitary Enterprise, State Scientific Center of Russian Federation, Research Institute of Atomic Reactors, Russia 2China Institute of Atomic Energy, Beijing Atomic Hi-Tech Corp., Ltd, Beijing, China Rheium-188 generators of ~1 Ci activity are the most prospective for clinical or centralized nuclear pharmacy use. One of the problems that have been poorly studied by now for that kind of generators is evaluation of generator's parameters stability during the long-term - for at least 6 month - operation. Results of performance study carried out for two experimental generators of ~1 Ci activity each are presented in the report. The study was implemented in 2002-2003 under the RIAR and CIAE joint research program. Tungsten-188 with specific activity of 3 Ci/g has been used for generators loading. Generator columns contained 7.8 g of acid alumina, columns were loaded from the saline with pH=3.5 at tungsten concentration ~20 mg/ml. One of the generators was stored in "dry" conditions, the second in the "wet" ones. Generators parameters - Re-188 yield, tungsten-188 breakthrough, radioactive impurities and aluminum content in the eluate - were measured periodically (each 1-2 weeks) using well know techniques. Besides, a scanning device was prepared providing study of tungsten-188 distribution along the generator column. For generator stored in a "dry" state yield of Re-188 was more than 90% during first two month of generator exploiting, than it

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decreased to 85% and was unchanged during next 220 days. For generator stored in a "wet" state yield of rhenium was lower, at ~75% level. Tungsten-188 breakthrough was found to be less than 10-6% after two initial generator washings, and was at the ~5.10-7% level thereupon, though, it was 2-3 units lower for the "wet" stored generator. Activity of radionuclide impurities (192Ir) was at the 10-5% level in the beginning of our experiments and more than one order lower afterwards. The aluminum content in eluate was less than 5 µg/ml during the first month, than it was a little bit higher - 7 µg/ml in average. It was demonstrated that tungsten-188 distribution along the generator column (distribution profile) changes during first 1-2 months of generator exploiting. After that distribution profile was stable, just slightly shifting to the lower part of the column. Results of the research have demonstrated that parameters of generators after their long-term exploitation were kept on the level, allowing their clinical use. 26 Production of radioisotopes in the BR2 high-flux reactor B. Ponsard SCK.CEN, BR2 Reactor, Mol, Belgium The BR2 reactor, put into operation in 1963 and refurbished in 1995-1997, is a 100 MW High-Flux "Materials Testing Reactor" which provides thermal neutron fluxes up to 1015 n/cm2.s. The production of radioisotopes, characterized by high specific activities, are carried out in dedicated in-core devices within standard irradiation cycles of 3 to 4 weeks and in accordance with a "Quality System" that has been certified to the requirements of the "EN ISO 9001: 2000" in November 2004. Due to its operating flexibility, its reliability and its production capacity, the BR2 reactor is considered as a major facility for a routine supply of radioisotopes such as 99Mo (99mTc), 131I, 133Xe, 192Ir, 186Re, 153Sm, 169Er, 90Y, 32P, 188W (188Re), 203Hg, 82Br, 79Kr, 41Ar, 125I, 177Lu, 89Sr, 60Co, 169Yb, 147Nd, ... Furthermore, various "test" irradiations are carried out to develop the production of new radioisotopes. Some irradiation devices allow the loading and unlaoding of irradiated targets during the operation of the reactor. Hot-cells and storage facilities are available to prepare and organize the shipment of the irradiated targets to dedicated processing facilities. 27 Production of high pure Einsteinium and Fermium preparations O.I. Andreyev, V.A. Tarasov, E.A. Zotov, A.Y. Baranov Federal State Unitary Enterprise "State Scientific Center of Russian Federation Research Institute of Atomic Reactors", Russia Highly pure einsteinium and fermium preparations are in the increased demand due to the progress in such fundamental and applied fields of modern sciences as nuclear physics and radiochemistry, nuclear medicine. The principal method of einsteinium and fermium production is irradiation of curium or californium isotopes in a high-flux nuclear reactor. Large-scale production of transplutonium elements at RIAR enables also to produce regularly significant quantities of einsteinium and fermium. In view of the fact that main routes for 255Es and 257Fm nuclear production are as follows: 252Cf(n,γ)253Cf(n,γ)254Cf(n,γ)255Cf(β-)255Es(n,γ)256Es(β-) 256Fm(n,γ)257Fm 252Cf(n,γ)253Cf(β-)253Es(n,γ)254gEs(n,γ)255Es(n,γ)256Es(β-) 256Fm(n,γ)257Fm curium targets irradiation is continued until 252Cf output reaches its peak value. Calculation results of einsteinium and fermium isotopes accumulation during irradiation of curium or californium targets in high-flux nuclear reactor SM are presented in the report. Used at RIAR the irradiated curium reprocessing procedure provides simultaneous extraction purification of californium, einsteinium and fermium from fission products and non-radioactive impurities. Subsequent separation of Cf-Es-Fm mixture is carried out by cation exchange chromatography using α-hydroxyisobutyric

acid (α-OHIBA) as eluant. Two fol-lowing purification steps of Es - Fm mixture from californium are usually needed before cation exchange separation and subsequent purification of the obtained Es and Fm prepara-tions are carried out. The purification procedure used allows reducing activity of 252Cf and fission products in ein-steinium preparations to a value less than 0.05 %. Depending on duration of the span between the end of irradiation (EOI) and isolation of einsteinium, the preparations with relative alpha activity of 253Es or 254Es above 99 % can be obtained. To obtain einsteinium preparation with increased 255Es content, trial irradiation of 253Es and 254Es mixture in the SM reactor was carried out. Possibility of regularly obtaining 255Fm preparations with radionuclide purity not less than 99 %, suitable for radiochemical research, was demonstrated experimentally. Laboratory research results as well as radiochemical procedures of irradiated targets processing and characteristics of obtained 253,254,255Es, 255Fm, 257Fm preparations are described in the report. Research was sponsored by INTAS (Project INTAS - 2000 - 00195) 28 Silicon doping installation at the new research reactor FRM-II X. Li1, H. Gerstenberg1, K. Fiederer2 1Technical University Munich, research reactor Munich FRM-2, Garching, Germany 2Hans Wälischmiller GmbH, Markdorf, Germany In contrast to the other irradiation facilities at the new reactor FRM-II, the silicon doping installation (SDA) is a production facility for enhancing the semiconductor material silicon (Si). High-performance electronic components in particular require their starting material Si to have a defined content of phosphorus (P) atoms distributed extremely homogeneously in the Si matrix. This doping is achieved by neutron capture and the resultant conversion of individual 30Si atoms into 31P with the P concentration in the Si being adjustable by varying the duration of irradiation. Our doping system is designed to allow the irradiation of cylindrical Si single crystals 500mm high and up to 200mm in diameter. To achieve the necessary axial doping homogeneity of ±5 %, the irradiation position is equipped with a nickel liner for vertical smoothing of the neutron flux profile and the sample is additionally rotated continuously about its own cylinder axis during irradiation. During irradiation, the neutron flux is controlled by four inline self-powered-neutron (SPN) detectors. The doping facility was tested and optimised by a test-rig during the start-up phase of the reactor. A major advantage of our doping system is the availability of a very pure thermal neutron field. Thus, parasitic threshold reactions by fast neutrons and the production of large clusters of irradiation defects are suppressed effectively. The maximal thermal neutron flux at the irradiation place is about 1.7E13 /cm²s. The ratio of the thermal to fast neutron flux is more than 1000. The exact irradiation position will be 15 cm vertically moved during the routine reactor cycle of 52 days, so that the SI-ingots are always located in the field with the maximal neutron flux due to the burn-up of the reactor. The final Si doping facility offering a semi automatic operation will be completed in the summer 2005 after the Ni-liner is optimised. It will be suitable for a production capacity till to 10 tons per year. Further, this doping system can be also used for the irradiation of large samples for example in the neutron activation analysis. Fig.1: Overview of the silicon doping facility at the FRM-II.

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Track 1 – Session 5: Isotope Production Cyclotron based 29 New cyclotron target for production of 67Ga and 111In I.E. Alekseev1, V.V. Darmograi2 1State University, Radiochemistry, St. Petersburg, Russia 2Central Research Institute of Structural Materials "Prometey", St. Petersburg, Russia For the industrial intrusion of diffusion-and-thermal methods of radionuclides separation [1] the new cyclotron target is offered. For the bombardment of metal Zn or metal Cd (production of 67Ga and 111In, basic diagnostic medical radionuclides) on exterior beams of the accelerators designed the cyclotron target in which the isotopic enriched materials is rendered on an inert tantalum substrate. For removal of heat during bombardment: a) on the part of a tantalum substrate the target is cooled by water, b) for cooling a obverse surface of a target the gaseous He will be utilized. The calculations are carried out: a) of the basic characteristics of a helium exchanger (for dissecting of irradiated target from volume of the accelerator the titanium or aluminium metal foils will be utilized), b) of strength of a tantalum substrate c) of temperatures of tantalum substrate and Zn (or Cd) targets at the bombardment by deuterons (energy - 13.5/0 MeV, beam current - 20 mA) or protons (energy - 16.0/0 MeV, beam current - 20 mA). [1] I.E. Alekseev Diffusion-thermal methods for recovering radionuclides from solid reactor and cyclotron targets: an outlook // Radiochemistry, 2003, Vol. 45, No. 5, pp. 429-456 (translated from Radiokhimiya). 30 Cyclotron yields of Rhenium-186 L. Solin1, V.A. Jakovlev1, I.E. Alekseev2, V.V. Lazarev3 1V.G. Khlopin Radium Institute, St. Petersburg, Russia 2State University, Radiochemistry, St. Petersburg, Russia 3State University, Nuclear Physics, St. Petersburg, Russia Energetic dependencies of 186Re yields under proton and deuteron irradiation of natural tungsten have been investigated by the "stacked foils" method. Energy range for protons was 16.5/5.3 MeV (cyclotron MGC-20) and for deuterons - 13.0/2.63 MeV (cyclotron U-120). Total 186Re yield for the proton energy of 16.5 MeV is equal to 0.85 MBq/µAh; in the case of 99%-enriched 186W target the 186Re yield can be increased up to 2.9 MBq/µAh. For deuteron irradiation of 13 MeV the yield of 186Re is 4.3 MBq/µAh; the 186W

enrichment up to 99% can increase the yield of the target product up to about 15 MBq/µAh. 31 Russian Sr/Rb-82 generator for PET investigations V. Chudakov1, B. Zhuikov1, P. Erilov1, L. Tyutin1, N. Kostenikov2, D. Ryzhkova2, E. Peterson3, D. Phillips3, J. Vincent3 1Institute for Nuclear Research of Russian Academy , Experimental Physics, Moscow, Russian Federat 2Medradiopreparat Co., Manufacturing, Moscow, Russian Federat 3Central Roentgen Radiological Research Institute, PET, Moscow, Russian Federat Sr/Rb-82 generator has been designed and fabricated by the Institute for Nuclear Research of Russian Academy of Science (INR) and loaded at Medradiopreparat Co. (Moscow). Accelerator produced strontium-82 (half-life of 25.3 days) adsorbed on a column decays to rubidium-82 (75 sec). Daughter rubidium-82 in chloride form is eluted from the column and injected with saline solution into patient's blood system. 82Rb decays yielding two 511 keV annihilation photons useful for Positron-Emission Tomography (PET) imaging. Sr/Rb-82 generator makes possible to perform myocardial perfusion heart studies [1]. Investigation of brain, stomach, kidney, lever, spleen and lung is perspective also. Starting isotope material strontium-82 is produced regularly at INR linear accelerator (intensive 100 MeV proton beam) and recovered chemically from irradiated targets of metallic rubidium at INR and Los Alamos National Laboratory. Inorganic sorbent comprising of amorphous α-hydrous tin oxide (particle size 80-160 µm) is produced by INR in Russia. The column shell (76 mm height, 22 mm diameter) has been designed basing on Canadian generator developed at TRIUMF (Vancouver) [2]. It is mainly made of standard stainless steel Swagelok parts including 25 µm filters (frits) and generator inlet and outlet lines with proper fittings. This design is reliable, strong and immune from radiation damage. The shielding container is made of tungsten alloy. Total weight is 20 kg, height - 275 mm, outer diameter - 95 mm. The sterile and non-pyrogenic eluent is isotonic saline (0.9% NaCl) with physiological pH (5.5-6.5) containing 82Rb with very low 82Sr and 85Sr contamination. At flow rate of 20 ml/min 82Sr breakthrough is 4.0·10-9 (total eluate volume 0.5 l) and 2.5·10-8 (total eluate volume 6.5 l) per ml of eluate. Other parameters of the generator are: "dead volume" is 4.5 ml; yield of 82Rb - not less than 70 %; total elution volume of saline is not less than 8.0 l. The main parameters of all produced generators of different activity (from 1 mCi to 100 mCi) appeared within regular requirements for intravenous preparation. The generator was tested at the Central Roentgen Radiological Research Institute (St.-Petersburg). The areas of infarction of rabbit heart were effectively determined at PET facility. The generator demonstrated high efficiency, reliability and simplicity in operation. The generator will be manufactured regularly in the near future. The work is supported by Initiatives for Proliferation Prevention Program (Project # T2-1093 LANL). References: 1. K.L.Gould. PET perfusion imaging and nuclear radiology. J. Nucl. Med., 1991, v.32, p.579. 2. M.R.Cackette, T.J.Ruth, J.S.Vincent. 82Sr Production from metallic Rb targets and development of 82Rb generator system. Appl. Radiat. Isot., 1993, v. 44, p. 917. 32 67Cu production techniques at Trace Radiochemical Inc D.J. Brown, J. Brawner, W. Courtney, J. Seals, H. Hupf, J. Medina Trace Radiochemical Inc, Denton, Texas, U.S.A. Trace Radiochemical is unique within the radiophar-maceutical and radiochemical industry in several regards. Firstly we are the only private linear accelerator in commercial production and second with the configuration of this Linac we can produce up to 6 different nuclides simultaneously. Moreover with the increased power (up to 70 MeV) we can exploit different excitation functions to better meet market demands with respect to quantity or quality and in the process reduce costs. For example we can produce 201Tl using a 205Tl target or 123I using natural iodine at higher energies as opposed to the current method utilizing a 203Tl or 124Xe targets. We are

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currently producing 67Cu (p,α) on at 70Zn target at 32 MeV, however we are in the process of increasing Linac power from 32MeV to 70MeV by adding two additional Drift Tube Tanks (DTL) Once complete, the reaction dynamics will change dramatically whereby we will use a 68Zn target using an optimal (p,2p) reaction to produce 67Cu at approximately 7 times the production rate of the p, alpha reaction or 0.459mci/µAmphr compared to 0.07 mci/µAmphr. 33 Production of Ga-66 from natural zinc A. Sattari, N. Shadanpour, G. Aslani, A. Rahiminejad Nuclear Research Center for Agriculture and Medicine, Cyclotron and Nuclear Medicine, Karaj, Iran In this study, production of Gallium-66 by irradiation of natural zinc target with 15 MeV protons was verified. Gallium-66 is an intermediate-lived radioisotope that has potential for positron emission tomography (PET), along study of the biological processes with intermediate to slow target tissue uptake. 66Ga (T½= 9.49; β+ (56.5%), EC (43.5%)) can be used in a large number of labeled proteins, peptides, and small molecules. We have produced 66Ga by irradiation of natural Zinc with 15MeV proton beam using the cyclotron (Cyclon 30) at nuclear research center for agriculture and medicine. A 400 µm Zinc target with copper backing substrate was irradiated for 1.5 hours with total integrated current of 250 µAh. Gallium has been purified from irradiated targets by passing through the cation exchange column and diisopropyl ether extraction. The concentration of Zinc and copper in 0.1 and 0.5 ppm were respectively measured by polarography. In order to detect impurities, gallum radioisotopes were detected by a Canberra HPGe gamma spectrometer. The production yield at EOB was 7mCi/µAh with total activity of 1.75 Ci for Gallium-66. The ratio of activity at 9 hours after the EOB for 66Ga(t½=9.5h), 68Ga (t½=1.1h) and 67Ga (t½=78h) was 98.63%, 1.12% and 0.25% respectively. The amount of 64Ga(t½=0.04h) and 70Ga(t½=0.35h) was not detectable. Due to using natural zinc, this method could be considered as an inexpensive method for laboratories studies. The production process comparing the irradiation of natural copper has no impurity such as copper-61, 64 and 67. The purification including cation-exchange and ether extraction afforded high yield beside negligible concentrations of copper and stable zinc as chemical impurity. Track 1 – Session 6: Carrier Free Isotope Production 34 Production of carrier-free reactor radionuclides using (n,p) and (n,α) threshold reactions Y.G. Toporov, V.A. Tarasov, F.Z. Vakhetov, V.T. Filimonov, O.I. Andreyev, A.S. Kornilov, R.A. Kuznetsov, Y.L. Revyakin, V.N. Kupriyanov, V.D. Gavrilov Federal State Unitary Enterprise State Scientific Center of Russian Federation, Research Institute of Atomic Reactors, Russia Using of threshold neutron reactions for reactor production of radionuclides allows, as a rule, producing of radionuclide preparations with specific activity close to the theoretical one. Sometimes, these reactions are the only approach available for production of particular products. A review of a list of radiochemicals - phosphorus-32,33, strontium-89, which are regularly produced by SSC RIAR using threshold (n,p) reactions is presented in the report. New developments of the Institute in the field of reactor radionuclides production using other threshold reactions are described in details. Results of experimental and calculation research of parameters of palladium-103 production under neutron irradiation of isotopically enriched cadmium-106 in the high-flux SM research reactor are presented. Procedures of palladium-103 isolation from irradiated targets as well as procedures for analytical control of the isolation process/purity of the palladium-103 are described. It has been found that depending on the irradiation conditions maximal yield of palladium-103 is 45+7 mCi/g for irradiation cycle of 40 eff. days. Effective cross-

section of the 106Cd(n,α)103Pd reaction was found to be 0,4 mbarn. Integrated yield of palladium-103 from one gram of cadmium-106 (till complete depletion of target material) was estimated to be 320-415 mCi. Quantitative dependencies of the yield and specific activity of 63Ni on irradiation time and position of the copper targets in the irradiation holes of the fast-flux reactor BOR-60 are presented. Procedures of 63Ni isolation from irradiated copper and purification from corresponding radioactive impurities are described. It was demonstrated that yield of 63Ni increases at irradiation time increase, specific activity of this radionuclide reaches its maximum practically just after beginning of irradiation and doesn't changes for very long time (for several years). Maximal specific activity value is determined by fast neutron spectrum and for positions in the active core of the BOR-60 reactor is 15 Ci/g. Calculations using multi-group model of the neutron flux density in the irradiation position and experimentally determined parameters of the product allowed one to evaluate the cross-section of the 63Cu(n,p)63Ni reaction that was found to be 6 mbarn. 35 Production of high specific activity 177Lu preparation using SM research reactor Y.G. Toporov, V.A. Tarasov, O.I. Andreev, E.A. Zotov, V.N. Kupriyanov, V.D. Gavrilov, A.O. Semenov Federal State Unitary Enterprise, State Scientific Center of Russian Federation - Research Institute of Atomic Reactors, Russia 177Lu radionuclide is of significant interest for modern nuclear medicine. To produce high specific activity 177Lu preparation such well-known methods as neutron irradiation of either 176Lu or 176Yb isotopic enriched targets may be used. The report shows the production yield of 177Lu and other nuclides assess the final product specific activity in respect of the SM high-flux nuclear reactor irradiation positions when thermal neutrons flux density is 1×1014 up to 2×1015 cm-2s-1. Maximum achievable specific activity of 177Lu produced via neutron irradiation of 176Yb strongly depends on a percentage of 175Lu, 176Lu, and 174Yb stable isotopes in the material to be irra-diated. The presence of 174Yb in ytterbium isotopes starting mixture results in decreasing 177Lu specific activity due to the following nuclear reactions: 174Yb(n,γ)175Yb(β-) 175Lu (n,γ)176Lu. Based on the nuclear calculation starting material quality specifications in respect of the content of these impurities have been determined. Laboratory research was carried out to develop radiochemical procedures providing 177Lu isolation from irradiated target, purification of 177Lu from ytterbium, radionuclide impurities and hafnium as the decay product. Purification of isotopic enriched ytterbium specimen (176Yb - 95.15; 174Yb - 2.47 at.%) from lutetium impurity followed by the irradiation in central neutron trap of the SM reactor were carried out. Electroreduction of ytterbium on Hg-cathode from lithium citrate solu-tion was used to isolate 177Lu from irradiated target. Cation exchange and extraction chromatogra-phy were used for further purification of 177Lu. Lutetium isotopic composition as well as ytterbium impurity content in 177Lu final prepara-tion were determined by mass-spectrometry and gamma-, X- spectrometry. 177Lu specific activity was calculated to be 9.27×104 Ci/g Lu (85% to its theoretical value) at the EOB. Long-lived 177mLu activity fraction did not exceed 1.4x10-4 % by that time. Total content of 176Lu and ytterbium iso-topes in final preparation is below the detectability limit for analysis techniques used, and so has no influence on 177Lu specific activity value. 36 Separation of microgram quantities of Lu-177 from milligram amounts of Yb by the extraction chromatography R. Mikolajczak, D. Pawlak, J.L. Parus Radioisotope Centre POLATOM, Research and Development, Otwock, Poland Extraction chromatography is an established technique for mutual separation of the rare earths elements at microgram level, which are met in the analytical applications. We present some results of the separation of microgram quantities of Lu from milligram amounts of Yb. This is a real situation when the carrier free Lu-177 is to be

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obtained by the irradiation of Yb-176 with neutrons in a nuclear reactor. Depending on the thermal and epithermal neutron flux of the reactor and the irradiation time and the enrichment of target material in the Yb-176 isotope, the weight ratio of Lu-177 to Yb is in the range from one to several thousands. We used the Yb oxide enriched to above 95% in Yb-176 which was irradiated in a neutron flux of 2×10E14 n/cm2s for about 100 hours. The Ln resin, 50 µm diameter grain size made by ®Eichrom was used as a separation medium and the HCl solution as an eluent. The separation column had length of 60 cm and a diameter of 0.9 cm. The separations were carried out at ambient and 50oC temperature. The solutions for separation with variable L/Yb ratios were prepared using the spikes of Lu-177 and Yb-169 obtained from neutron irradiation of the defined amounts of Lu and Yb of known isotopic composition. The results of several separation runs with the different Lu to Yb ratios will be presented showing the separation yield of Lu as a function of this ratio and the load of the column. The volumes of the Yb and Lu fractions are of a few hundred milliliters hence the reduction of volume through evaporation is necessary. This process increases the concentration of inactive impurities such as Fe, Cu and Zn, which are very competitive in the Lu-177 labelling of chelators used for radiopharmaceuticals. Detailed discussion of the impurities problem will be given and the remedial actions will be indicated. 37 Deuteron-induced reactions onf Yb: a carrier-free alternative to reactor-produced 177 Lu? A. Hermanne1, E. Lavie2, M. Goldberg2, S. Takacs3 1Vrije Universiteit Brussel, Applied Physics - Cyclotron, Brussels, Belgium 2Soreq NRC, Medical Applications, Yavne, Israel 3Atomki, Debrecen, Hungary The use of radiolabeled biomolecules, such as peptides and monoclonal antibodies, for therapy applications is a fast growing field in nuclear medicine. The radionuclide 177Lu (β- of 497 keV (78.6%), T½= 6.7 days) has excellent properties for therapy. At present, 177Lu is produced in reactors by neutron-capture on natLu or enriched 176Lu. However, since efficient labeling of the biomolecules requires very high specific activity, production is confined to high-flux reactors. To increase availability of 177Lu, we investigated the possible production of high activity, carrier-free batches by deuteron induced reactions on Yb-targets with an accelerator. Two stacks of natYb (12µm thick) were irradiated at the cyclotron of the VUB with deuteron beams of 21 and 15 MeV respectively. High purity Ti (10µm) monitor foils were interleaved and allowed accurate assessment of beam intensity and energy degradation. The time-sequence of g-measurements of induced activities shows that the principal contribution to 177Lu production is the indirect reaction 176Yb(d,p)177Yb (T ½= 1.9 h, decaying via β- to 177Lu). The cross section for this reaction attains a maximum of 26 mbarn at Ed= 11 MeV and exhibits a tail extending beyond 25 MeV. The data show that direct feeding via the 176Yb(d,n)177Lu reaction has a cross section that is measurable only above 12 MeV and does not attain a maximum in the energy range studied. Hence production of 177Lu is only significant via formation and subsequent decay of 177Yb. The favorable ratio of half-lives permits obtaining carrier-free 177Lu from Yb targets in irradiations of up to several days duration, followed by chemical separation. To increase the overall 177Lu yield and to eliminate contamination with 170,171,172,173Lu, highly-enriched 176Yb should be used. From fits to our excitation curves, thick-target yields have been computed. Batches of 30 Gbq of 177Lu can be produced in 72 h irradiations with 21 MeV deuterons (100µA beam, 100µm thick enriched targets). This value does not compare favorably with production at high flux reactors, where batches of 3700 Gbq using natLu are reported (7 days irradiation at a thermal flux of 3 x1013n/cm2/s, using 100mg of material, the cross section for 176Lu(n,γ)177Lu being 2100 barn). However the prospect of obtaining carrier-free 177Lu in accelerator-based productions, could present significant advantages for the application in question

38 "Direct" production of lutetium-177 (Lu-177) from enriched Lu-176 in a high flux reactor - the only practical route to provide high multi curie levels of high specific activity Lu-177 required for routine clinical use F.F. Knapp1, S. Mirzadeh1, A.L. Beets1, M. Du1, J.A. Klein2, M. Garland3 1Oak Ridge National Laboratory, Nuclear Medicine Program, Oak Ridge, U.S.A. 2Oak Ridge National Laboratory, Isotope Program, Oak Ridge, U.S.A. 3University of South Carolina, Department of Mechanical Engineering , Columbia, U.S.A. Increasing interest in targeted therapy with high-specific-activity (HSA) Lu-177 (t1/2 = 6.71 d; β Emax 0.497 MeV; γ 208 keV, 11%) requires routine availability of high multi-Curie levels at reasonable cost. Lu-177 (theoretical SAmax = 110 Ci/mg) is reactor-produced by either the “direct” Lu-176(n,γ; σ = 2090 barn) Lu-177 route or the “indirect” Yb-176(n,γ; σ = 2.85 barn)Yb-177(t1/2 1.9 h; β-→)Lu-177 method, with low-level Lu-177m (t1/2 = 160 d) contamination. We evaluated both "direct" and "indirect" Lu-177 production yields in the ORNL High Flux Isotope Reactor (HFIR). We estimated HSA Lu-177 Ci/mg Lu-176 using the LAURA code at the following 2200 m/sec flux values: 2.0 x 1015 neutrons/cm2/sec (i.e. HFIR or SM Reactor), 78 Ci/mg (4 d); 4 x 1014 (i.e. MURR), 32 Ci/mg (11 d); 1 x 1014, 13 Ci/mg (20 d). HSA Lu-177 is thus uniquely directly produced in high flux reactors and depends on the thermal neutron flux, irradiation parameters, target enrichment, etc. Experimental HFIR values are ~75 Ci/mg after 3-4 days irradiation (Lu-117m/Lu-177 ~10-5). The “indirect” route could provide no carrier added (n.c.a.) Lu-177 free of Lu-177m, but Yb-176 procurement/recovery costs, low Yb-177 production yields, large target volume requirements, decay losses during processing and purification, etc., must be assessed. “Indirect” HFIR Lu-177 yields (9-10 days) are only about ~300 mCi Lu-177/mg Yb-176 (~250 fold lower than “direct”), thus requiring effective Lu-177/Yb separation. For production at lower flux, significantly lower Yb-177 production yields are expected. After HFIR irradiation, we separated Lu-177 from Yb by acid elution of Eichrome Ln resin. Processing and dispensing of Lu-177 from the “direct” route is straight forward and efficient, while processing and purification from the “indirect” route is time consuming and expensive. High multi-Curie levels of HSA Lu-177 could not be practically produced by the "indirect" approach, because of much lower yields, costly and time consuming chemical processing and expected generation of large volumes of radioactive waste. The large multi-Curie levels of HSA Lu-177 required for clinical use could only be cost-effectively routinely produced by the “direct” route in a high flux reactor such as the HFIR with capabilities for on-line access to the reactor core. ORNL is managed by UT Battelle, LLC, for the U.S. Department of Energy, under contract No. DE-AC05-00OR22725. 39 A new method for the production of carrier-free 103Pd R. Hubert, F. Bodart, S. Lucas University of Namur(FUNDP), Physics, LARN, Namur, Belgium Nowadays, the number of patients suffering from prostate cancer treated by brachytherapy is increasing. 103Pd can be used for this therapy; it offers attractive properties like its short half-life and its low energy emission. The carrier-free 103Pd can be obtained in two steps: production by the 103Rh(p,n)103Pd reaction in cyclotron and extraction from the Rh matrix. 103Pd is actually extracted by wet chemical method that has disadvantages: expensive and complex due to multiple stages of chemical procedures, waste production. Another method largely used by Beyer and al. within the scope of ISOL targets for the production of radioactive ion beams was studied. It consists in annealing the Rh irradiated target under vacuum. By diffusion and evaporation 103Pd is extracted keeping the Rh in a solid form. The activated Rh samples used were Rh coils of a 50µm/ 200µm section irradiated with a 14MeV proton beam, activity reached was approximately 1mCi/cm. These coils were annealed in a tubular furnace under vacuum at different

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temperature from 1100°C to 1500°C. 103Pd extraction curves were deduced, effects of pressure, annealing time and sample thickness were investigated. All the results will be analysed and discussed. 40 Isolation of carrier-free radioisotopes of some transition elements in the form of volatile chlorides, chalkogenides and pnictides V.P. Domanov Joint Institute for Nuclear Research, Dubna, Moscow, Russia The developed gas-chemical procedures of isolation of some carrier-free radioisotopes are presented. A thermochromatographic (TC) technique was used in the majority of the cases. For isolation of the desired products, they were converted into volatile chlorides, chalkogenides or pnictides, transported from the starting zone in a stream of purified helium along the open-tubular quartz TC column and adsorbed on its walls at certain temperatures. Their positions are defined by γ-spectrometric measurements. Methods for efficient separation of components of some generator pairs in the gas phase are also presented. As a rule, a daughter radionuclide is periodically isolated from a parent one. An alternative approach is proposed. The components of the 172Hf-172Lu generator pair were converted into waterless chlorides and were separated in the TC regime. Volatile 172HfCl4 was deposited at ~200°C and LuCl3 remained in the starting zone of the TC column and could be extracted. After accumulation of 172Lu the adsorbed fraction of the parent activity was placed in the starting zone and the process could be repeated. Analogically, components of the 44Ti-44Sc pair were transformed into chlorides, volatile 44TiCl4 was evaporated and unvolatile 44ScCl3 was collected in residuum. Special equipment was developed to repeat the procedure. Vapors of S, H2S, Se, Te, P, As and Sb were used as reagents to produce volatile compounds of other transition elements. The products of nuclear reactions Hg +p and Cd+p (660 Mev) were heated at 900°C in a stream of He, containing a gaseous reagent. In the presence of S vapor 99Mo formed a volatile sulfide that was adsorbed at 280°C (the yield was equal to 85%). At the same time, with H2S as a reagent, a selective isolation of 183,184Re at 300°C (80%) was performed. 100,103Pd was adsorbed at 550°C (60%) at the presence of Se vapor. 188Pt was isolated at 640°C (70%) at the presence of Te vapor. It is shown that Au and Ag form volatile pnictides. 195,196Au in the presence of P vapors was collected at 660°C (65%) and in the presence of As vapor aurous arsenide was formed which was adsorbed at 770°C (30%). At the presence of Sb vapor 105,106Ag was selectively isolated at 750°C (50%). Compositions of the formed compounds are discussed. The γ-spectrum of the isolated fractions indicates their high radiochemical purity (at the most part at the level 99.9%). The isolated radioisotopes can find application in science and technology, in partucular, 99Mo and 188Pt radioisotopes can serve as a source of production of the daughter activity 99mTc and 188Ir respectively. Three of presented methods are protected by author's right. Track 1 – Session 7: Stable Isotopes 41 Production of stable isotopes utilizing the plasma separation process T.S. Bigelow, F.J. Tarallo, N.R. Stevenson Theragenics Corporation, Oak Ridge, USA The Plasma Separation Process (PSP) has been reassembled and is operational in Theragenics Corporation's® Oak Ridge, TN, facility. The PSP was formerly used in the U.S. Department of Energy's (DOE) Advanced Isotope Separation program, and is being leased by Theragenics™ from the DOE. The PSP utilizes mass discrimination to separate stable metal isotopes and is believed to be the only such process of its scale currently in operation. Key portions of this process include a microwave system that provides electron cyclotron resonance heating to form the plasma, an ion cyclotron resonance frequency system used to excite the desired isotope mass, and a 44-ton superconducting magnet capable of

generating a magnetic field of up to 2 tesla. The PSP is designed to separate relatively large quantities of stable metal isotopes at moderate to high enrichment levels, and is capable of separating almost all isotopes of metallic elements. System and operational improvements are being considered that could increase throughput and enrichment capabilities. Theragenics™ also has laboratory and analytical facilities at the PSP site capable of harvesting the isotopes from the process and analyzing enrichment. Since becoming operational in 2002, Theragenics™ has utilized the PSP to separate isotopes from the following elements: dysprosium, erbium, gadolinium, molybdenum and nickel. Currently, Theragenics™ is using the PSP for the separation of 102Pd, which can be used as precursor for the production of 103Pd. The 103Pd radioisotope is used in TheraSeed®, which is Theragenics'™ medical device used primarily in the treatment of early-stage prostate cancer. Theragenics™ also has research and development programs underway utilizing 103Pd for the prevention of restenosis and the treatment of certain types of macular degeneration. Other industrial, medical and research opportunities are also being considered using other isotopes. The opportunities for beneficial uses of isotopes is enhanced with the capabilities of the PSP, possibly including applications that may have previously been overlooked or rejected as being impractical. In addition to Theragenics'™ operational experience to date, potential PSP applications and capabilities will be discussed. 42 Centrifugal technology for stable isotope separation at the electrochemical plant A.N. Shubin1, G.M. Skorynin1, E.A. Nikitina1, I.A. Okhotina2 1The Production Association "Electrochemical Plant" (PA "ECP"), Russia, Krasnoyarsk Region, Zelenogorsk 2The Federal Agency for Atomic Energy, Russia, Moscow Almost one third of enrichment capabilities of Russia is concentrated at the ECP, with the start-up of which in the 1960s the formation of a complex of four enterprises was completed to produce highly enriched uranium in the USSR. Early in the 1970s, after the estimated uranium enrichment capabilities of the enterprise had been achieved, the ECP started commercializing a stable isotope separation process. At present the enterprise is a research-and-production complex including two design departments which are situated in Saint-Petersburg and Nizhni Novgorod and develop gas centrifuge designs for separation of isotopes of uranium and other chemical elements. For the last three decades isotope separation technologies for more than 20 chemical elements have been commercialized at the ECP. A brief history of the development of centrifugal technology is presented in the report. It reflects the role of the leading scientific institutions and organizations (RRC "Kurchatov Institute", MSEPI (TU), UEIE, etc.) in providing a basis for separation theory and in pursuing experimental investigations. Cardinal scientific and technical problems, related to process substance peculiarities used to separate isotopes of different chemical elements in gas centrifuges, are discussed. Particularly, the necessity is mentioned to consider the effects caused by polyisotopy of atoms forming process gas molecules: multi-component mixtures, isotope "overlapping", isotope exchange. The enterprise development dynamics both for stable isotope capability and isotopic product range, examples of the use of such products in science, technology and medicine are given. The international science projects for which the ECP has supplied or will supply stable isotopes are listed. The record concentrations of someisotopes that were achieved in pilot batches production are indicated. Stable isotopes are produced by pilot facilities in Saint-Petersburg, Nizhni Novgorod and special-purpose workshop at the basic enterprise in Zelenogorsk, where industrial isotope production is called "SVETLANA". The analysis of stable isotope world market demonstrates that the ECP products take up a well-deserved position in it. Work on the development of the technology, the development of new gas centrifuge modifications and expansion of the range of isotopic products is constantly carried on at the enterprise. The ECP production capacity and the advantages of the technology provide a

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possibility of executing substantial orders for stable isotopes applied in various spheres of people's activity. 43 Pecularities of laser photochemical isotope separation using long-living states P.A. Bokhan, D.E. Zakrevsky, N.V. Fateev Institute of Semiconductor Physics, Siberian Branch, Russian Academy of Science, Novosibirsk, Russia Basically laser isotope separation method has been followed two main directions. The first one is a selective multistep excitation of atoms in atomic beam, followed by electrostatic extraction (AVLIS). Second one is multistep photodissociation by means of powerful infrared radiation. Photochemical method, which based on selective atom (molecule) excitation followed by chemical reaction, has not been developed. In the present report the main results of photochemical laser isotope separation method are propounded. The essential features required for working particles, gas-reagent and radical acceptor are formulated. The main advantages and disadvantages are considered. The first ones are as follows; a) high concentration of working particles in separating chamber (up to 1013 cm-3); b) - one photon excitation; c) - usage of gas stream; d) - simple product extraction. As an example separation of Zn and Rb isotopes has bean demonstrated. It was shown that using of long-living states is critical requirement for efficient isotope separation. Otherwise high concentration of reagent is necessary to realize high quantum yield. Because of broadening of absorbing line it followed by the selectivity decrease making difficult to organize rapid stream of operating mixture and product extraction. The main peculiarities of lead isotope separation are considered. It is supposed that 204,206Pb may be the best environmentally safe coolant for power reactors with fast neutrons. This task is practically ideal one for laser photochemical method because a lead atom has high energy metastable states. These states can be excited by high efficient turnable diode lasers. It makes possible considerably to decrease the separation cost. This task has been developed under International Science and Technology Center support, project #2573. 44 Production of carbon and oxygen isotopes in RRC "Kurchatov Institute" G. Grigoriev, I.P. Gnidoi, A.A. Dyatlov, A.T. Peshkov, A.L. Ustinov Russian Research Center "Kurchatov Institute", Institute of Molecular Physics, Moscow, Russia The Institute of Molecular Physics of RRC "Kurchatov Institute" is one of the biggest producers of stable isotopes. It has developed centrifuge, photochemical and laser technologies of isotope separation. Many years it has no technologies for separation of light isotopes. Now two installations for production of carbon and oxygen isotopes is designed, assembled and launched into operation. Separation of carbon isotopes is based on a method of cryogenic rectification of carbon oxide. The carbon complex consists of the three separation modules, system for carbon oxide purification, control system of input and draw-off flows, gas, vacuum and compressor equipment, system of the automatic monitoring and control of the complex. The two-step cascade with height of packed columns about 40 meters is realized in first module. Second module has three-step cascade and scrambler for normalization of oxygen isotopes content. Third module is designed for enrichment of product that is preliminary enriched to 30% by laser method. Separation of oxygen isotopes is based on a water distillation at low pressure. Water complex consists of four-step separation cascade of separation columns with different diameters, system of water preparation, cooling system and system of the automatic monitoring and control of operation. In this report the results of operation of these installations are presented.

45 Application of stable isotopes in a basic nuclear physical research V. Baranov, G.Y. Grigoriev Russian Research Center "Kurchatov Institute", Institute of Molecular Physics, Moscow Isotopes in general and stable isotopes are very important instruments in a basic nuclear physical research, especially in investigations of physics of weak interactions. From the point of view of nuclear physics the isotopes of the same element differ not only and not so much on weight of a nuclear nucleus, but they are different on the properties shown in nuclear reactions. These properties arey very important for radioactive isotopes production, nuclear labeling and nuclear interactions. Some of the stable isotopes are not "very stable" and can decay through double beta process but at very low probability. Investigations of double beta decay can discover very important properties of matter such as neutrino mass limit. Because of very rare events of double beta decay and especially neutrinoless double beta decay it is necessary to use very big amount of stable isotopes that can show such kind of decay. Existing and planning experiments and possibilities of production of necessary amount of isotopes are reviewed in this report. 46 Thermal conductivity of silicon-28 and separation technologies for its production V.D. Borisevich1, A.V. Khoroshilov2, S.A. Cherednichenko2 1Moscow Engineering Physics Insitute 2D.I. Mendeleev University of Chemical Technology, Moscow, Russia The knowledge of thermo-physical properties of materials used in the electronic industry plays a crucial role in the design process of electronic devices and integrated circuits. First, in experiments it has been demonstrated that silicon enriched with the Si-28 isotope possesses bigger thermal conductivity than silicon of a natural abundance. It allowed to believe that Si-28 could become a revolutionary semiconductor material because it may provide an elegant way to address thermal problems since its benefits can be obtained without radical changing existing technology. These results had no good enough correlation to the theory. So the reliability of the experiments has been called in question and the new much lower results in the thermal conductivity of Si-28 have been obtained. Recently, the new experimental data have indicated a gain of approximately 55% in the thermal conductivity of highly enriched Si-28 to that of natural silicon at room temperature. It is stimulated a new stage of theoretical and experimental works on separation methods for large-scale production of Si-28. The paper contains the analysis of the theoretical and experimental results on application of separation methods from two groups (physical and physical chemical ones) to enrichment of Si-28. The specific features of Si-28 application in a semiconductor industry have led to understanding the necessity to provide not only isotopically pure silicon, but to meet all requirements in purity of a final substance for production of electronic devices. Studying separation methods from the first group, the concern was, in particular, to ascertain the influence of usage of tetrafluoride of silicon (SiF4) and trichlorosilane (SiHCl3) as a process gas in a gas centrifugation process for concentration of Si-28 taking into account either separation problems or manufacturing benefits. Trying to understand the problems come across in so-called classical separation methods from the second group, we have obtained the new experimental data on separation silicon isotopes by the chemical exchange method using the SiF4 - SiF4A-type working systems, where A is a complex-forming agent. The information accumulated has been used as a basis for a comparative analysis of two mentioned above groups of separation methods. Finally, using the special technique, it was calculated a cost price of highly enriched Si-28 that the chemical exchange and gas centrifuge methods in large-scale manufacturing can provide.

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Track 1 – Session 8: Waste and Transmutation 47 The Dovita Transmutation program - Results of the 10-year activities RIAR (Dimitrovgrad) A. Bychkov, O.V. Skiba, A.A. Mayorshin, M.V. Kormilitsyn, O.V. Shishalov, I.Y. Zhemkov RIAR, Dimitrovgrad-10, Romania Since 1992, SSC RIAR has proposed the demonstration program-concept DOVITA (Dry reprocessing, Oxide fuel, Vibropac, Integral, Transmutation of Actinides), which should demonstrate opportunities of new technologies for realization of the optimized fuel cycle for actinide burner reactor (for transmutation of Np, Am, Cm). RIAR use BOR-60 reactor as the experimental base for carrying out of DOVITA Program investigations, because highly hardness of BOR-60 neutron spectrum is very beneficial for minor actinides burning. The flow sheet of fuel production and reprocessing provides homogeneous option for neptunium recycle in MOX fuel. It is preferable to introduce americium and curium into special targets. Fuel recycle is carried out by the following flow sheets: - The basic (driven) MOX fuel, after 15-20 % burn-up, is underwent to decladding, crushing, vacuum reprocessing and repeated vibropacking; - After two cycles of irradiation, the basic fuel is reprocessed by pyroelectrochemical methods. U, Pu and Np (and portion of Am) come back to irradiation; - The materials of targets with Am, Cm and REE are irradiated by 3-4 cycles with periodic decladding and treatment, then they are directed to pyrochemical process; - The pyrochemical process of Am and Cm separation from REE will be carried out in system with liquid metal electrode, thus the REE portion is dumped only. The step-by-step work is carried out for the criteria choice, description and substantiation of DOVITA fuel cycle concept on the basis of the data. The ABFR fuel cycle differs essentially from the fuel cycle of thermal neutron reactors. It is caused by it is inexpedient to release FPs from fuel containing minor-actinides and plutonium up to high decontamination factors, because its activity is determined mainly by actinides radiation. As result it is necessary to realize all operations with fuel in remote conditions. ABFR closes a fuel cycle of nuclear power as a whole, so the special requirements must be presented to amount and form of radioactive wastes formed in its external fuel cycle. Besides, taking into account a lower economic efficiency of ABFR in comparison with power reactors, the fuel manufacture should be cheap and compact. This approach to the decision of ABFR fuel cycle problem is based on experience and knowledge obtained during development of the fuel cycle with application of pyroelectrochemical (and other "dry") methods for fuel reprocessing and production and vibropacking method for fuel pins manufacture: - The main parameters of obtaining the (U-5%Np)O2 granulated fuel by the electrolysis in melted salts, as well as the physico-mechanical characteristics of the granulate, have been studied. The fabricated by the vibropack technology fuel pins were irradiated in the BOR-60 reactor up to the burn up of about 13 and 20 % h.a. The batches of UO2- 20%PuO2- (3-6)%NpO2 fuel have been produced and the physico-mechanical and physico-chemical properties of their components have been investigated. Fabrication of vibropack fuel pins containing this fuel is scheduled for the 2003 - There have been obtained four products with weights within the range from 50g to 70g, americium content of 2-3 % wt and plutonium content over the range from 2 to 50 %. Now these products are being investigated and prepared for irradiation in BOR-60 reactor. - There have been performed demonstration experiments on pyroelectrochemical treatment of MOX-fuel with burnup 4,7% h.a. for BN-350 reactor (1991 -1992) and with burnup about 21-24% h.a. for BOR-60 reactor (1995 -1996). During the experiments MAs behavior has been controlled. - Two pins including eight ampoules containing pure actinides are irradiate in BOR-60 reactor since

December 1998 for the adjustment of nuclear physical constants. In October 2001 the irradiation of one pin was finished. Now irradiated ampoules are under investigations by radiochemical and mass-spectrometry methods. On the basis of the above proposed flow-sheets and RIAR experience the layout and scheme of the Pilot Plant are developed for ensuring of the external ABFR fuel cycle. The primary evaluations of operational and capital expenses are carried out. The DOVITA program is not completed yet. However, the researches fulfilled during 10 years have shown that the main part of problems connected with the ABFR fuel cycle can be solved. The complex decision of minor-actinide recycle problem is possible without creation of new exotic systems, and only on the basis of known technological methods and with application of known reactor systems. The complex study on chemical aspects of the program (manufacture and reprocessing of fuel) would be completed during nearest 2-3 years. It is planned to finish the demonstration reactor experiments during further 4-5 years. The future R&D plans of SSC RIAR include a widening of researches on various fuel compositions for radiotoxical actinides transmutation. References: 1. Bychkov A.V., Mayorshin A.A., Skiba O.V. The Proposed Fuel Cycle of The Actinide Burning Reactor - DOVITA./ Proc. of Specialists Meet. "Use of Fast Reactors for Actinide Transmutation" Obninsk, 22 24 Sept.1992. IAEA TECDOC 693. IAEA, Vienna, 1993, p.118. 2. O.V.Skiba et al. Technology of Pyroelectrochemical Reprocessing and Production of Nuclear Fuel. Proc.Int.Conf. GLOBAL'93, 1993, Seattle, ANS, 1993, v.2, p.1344. 3. A.V.Bychkov, M.V. Kormilitzin et al. Development of the pyroelectrochemical process for demonstration fuel cycle of an actinide burner reactor. / Proc. Int. Confer. on Evaluation of Emerging Nuclear Fuel Cycle Systems. GLOBAL'95. Sept.11-14,1995.Versailles. v.1, p.516. 4. M.V.Kormilitzyn, A.V.Bychkov et al. Application of Pyroelectrochemical Methods for Production of the Fuel Composition (U,Np)O2, (U,Pu,Np)O2, (U,Am)O2 in Molten Chlorides. / In: "4th Int.Conf. on Nucl.and Radiochemistry, NRC4. St.Malo, France, 8-13 Sept.1996. Ext. Abstracts". 1996. Vol.2. r.G-08. 5. A.V.Bychkov et al. Pyrochemical Reprocessing of Irradiated Mixed Oxide Fuel in Molten Salts. Molten Salt Forum. Proc. 5th Int. Symp. on Molten salt Chemistry and Technolgy, Drezden, Aug.21-25, 1997. 6. A.V.Bychkov et al. Fuel Cycle of Actinide Burner Reactor. Review of investigation on DOVITA Program. Proc.Int.Conf. GLOBAL'97. Yokohama, 1997, v.1, p.657. 7. V.B.Ivanov et al. Experimental, Economical and Ecological Substantiation of Fuel Cycle based on Pyrochmical Reprocessing and Vibropac Technology. Proc.Int.Conf. GLOBAL'97. Yokohama, 1997. v.2, p.906. 8. Bychkov A.V., Vavilov S.K. et al. Pyroelectrochemical reprocessing of irradiated FBR MOX fuel. III. Test on high burn-up BOR-60 fuel. / Paper on GLOBAL-97 Conferences, 5-10 Okt., Yokohama,. Japan. 9. A.A.Mayorhsin, V.A.Kisly, O.V.Shishalov et al. Calculative-experimental validation of minor actinides transmutation in the bor-60 reactor. Experience on vibropac UNpO2 fuel irradiation./ GLOBAL 2001 international conference "Back-end of the fuel cycle: from research to solutions" Paris, France, 9-13 Sept. 2001 48 To the possibility of transmutation of minor actinides at high-current low-energy electron accelerators D. Kamanin1, A.A. Goverdovski2, A. Matthies1, A.D. Rogov3 1JINR, FLNR, Dubna, Russia 2IPPE, DNNP, Obninsk, Russia 3JINR, FLNP, Dubna, Russia Main minor actinides are characterized by so-called threshold fission cross-section and therefore their transmutation can be reached utilizing only a small fraction of neutrons available in power reactors. The use of bremsstrahlung rays from a thick W-converter target irradiated with 20-30 MeV electrons can provide a much more effective transmutation effect due to the specific shape of cross-sections around the giant resonance. Our direct calculations demonstrate that there is a real possibility of using "low" energy electron accelerators for solving the nuclear waste problem in an efficient way. In particular, the total transmutation efficiency of Np-237 can be more that 50 kg per year for 1 GWt of power. This value is comparable with those for fast or thermal nuclear power reactors (70-140 kg).

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49 Management of radioactive waste resulting from radioisotope production on the IRE Site Y. Niels, V. Host, M. Baccus, P. Raty National Institute for Radioelements (IRE) , Fleurus, Belgium Different companies operating on the IRE site, are producing radioisotopes for medical and industrial use and are generating low and medium level radioactive waste mainly contaminated with short lived isotopes. IRE waste department is in charge of the management of the different waste streams and has developed specific procedures for taking benefit of the specific decays, before final disposal of the waste. The management of the solid waste is performed in a new dedicated building which includes unique design features. For the medium level waste coming from the production lines, optimal management is performed in installations including the following specific equipments: - 2 hotcells highly shielded for receiving waste packages showing a dose rate up to 400 Sv/h - A shielded turntable storage which can accommodate 800 waste containers for decay for months or years. - An integrated measurement device for the follow up of the decay of the containers dose rate. - A specific ventilation and monitoring system of the installation for coping with contaminations including radioactive iodine. After measurement of the decay below a 2mSv/h dose rate level, the waste containers are pressed and packaged in 200 litres drums which will be further considered as low level waste. For the low level waste coming from the laboratories, the installation includes two spectrometry monitoring systems for performing accurate quantification of gamma emitters contained in the packages. On the basis of the measurement results, the appropriate disposal solution can be selected, either as radioactive waste or as industrial waste if the activities are below the clearance level fixed by the National Authority. In addition and in order to assess the non measurable activities (for pure α or β emitters) which vary broadly versus the origin of the waste, a strict traceability program has been put in place. For insuring the optimal safety for these operations, most of the handling and measurements steps have been automatised and are recorded whereas the buildings and the equipments are continuously monitored, in real time, both with regards to radiological and process parameters. The computerized supervising system allows to control, visualizes and records all the functional parameters of the installation. 50 Transmutation and fusion of anomalous and exotic stable and radioactive isotopes S.V. Adamenko1, A.S. Adamenko1, V.I. Vysotskii1,2 1Electrodynamics Laboratory "Proton-21", Kiev, Ukraine 2Kiev Shevchenko National University, Faculty of Radiophysics, Kiev, Ukraine The results of experiments on abnormal stable isotopes production during process of direct transmutation of monoatomic targets and on direct deactivation of radioactive isotopes up to stable state in Kiev Electrodynamics Laboratory "Proton-21" are presented. The method of reactivation does not use neutrons or particles of high energy. The theory of the deactivation process is also discussed. During 2000-2004 more then 10000 experiments on superpressing to a collapse state of monoatomic solid density targets by a special electron driver were carried out in the Laboratory. Investigations were carried out at different coherent exposure conditions with various targets of controlled composition, made of light, medium and heavy both stable and radioactive elements with atomic masses 12< A< 210. All together, more than 17000 element and isotope analyses were performed, including the following: EPMA, LMS, AES, SIMS, TIMS, RBS. In each of these experiments several types of anomalous phenomena were observed: a) fusion of light, media and heavy elements (at 1 ≤A<240) with abnormal isotopic ratios;

b) fusion of superheavy transuranium elements (about 1014-1015 superheavy nuclei were created in each of the performed experiments); c) all created elements and isotopes (including superheavy ones) were stable or quasistable (including the case when initial target was made of radioactive isotopes); d) transmutation of any radioactive targets to stable-nucleus states in the collapse zone. These phenomena with a high probability can be interpreted on the basis of the main common idea - creation and evolution of a self-organized and self-supported collapse of electron-nuclear plasma of initial solid-state density under the action of focusing electron driver up to a state of large nonstationary electron-nuclear giant cluster with density close to that of a nuclear substance. In such cluster the process of prompt transmutation of all radioactive nuclei to different stable isotopes take place. The duration of transmutation in any case less than 10-9 s. A principally new approach to the creation of superheavy nuclei based on the stimulation of a self-organizing collapse of electron-nuclear systems is also analyzed [1]. For a neutral atom compressed by external forces, a threshold electron density is shown to exist. If such a density is reached, a self-organizing process of "electron downfall to the nucleus" starts. This process is exoenergic and leads to the formation of a supercompressed electron-nuclear cluster. The higher the charge of a nucleus, the lower the threshold of the external compression. It is shown that the maximum binding energy shifts during such a self-organizing collapse of the electron-nuclear system from Aopt = 60 (for uncompressed substance) to the area of high mass numbers Aopt = 200-2000 and could render the synthesis of superheavy nuclei to be energy-efficient. The synthesis proceeds through the absorption of other nuclei by the collapsed nucleus. It is theoretically proved that the synthesis efficiency is ensured by both the width reduction and increased transparency of the Coulomb barrier in the extremely compressed electron-nuclear system. The release of binding energy through the absorption of radioactive nuclei by the electron-nuclear collapsed clusters may result in the simultaneous emission of lighter stable nuclei (fusion-fission processes). The experimental value of the utilization efficiency of radionuclides per 1 kJ of the electron driver energy corresponds to the transmutation of about 1018-1019 radioactive target nuclei of any kind (e.g., 60Co, 137Cs) into nonradioactive (stable) isotopes of other nuclei. The coefficient of deactivation of radioactive nuclei to stable ones in zone of transmutation equals to 100%. [1]. S.V. Adamenko, V.I. Vysotskii, Foundations of Physics Letters, 17, 203 (2004). 51 Determination of absorption characteristics for different Cs selective resins J.R. Zeevaart1, S.A. Shady2, A. Goede1 1Necsa, Radiochemistry, Pretoria, South Africa 2Atomic Energy Authority, Nuclear fuel technology, Cairo, Egypt Cs-137 is often used for industrial and medical gamma sources. These sources could consist of Cs-137 which is adsorbed on inorganic or organic resins, preferably vitrified to form a fixed source. Furthermore Cs-137 is also one of the isotopes to be removed from high level radioactive liquid waste in a economical and safe manner. Combining these objectives a study was embarked on to evaluate the adsorption capacity of five different commercial resins. Kd values of the five resins for Cs (using Cs-137 as a tracer) were determined which reduced the further investigations (capacity and exchange rate) to three resins. The resins investigated are, according to the literature, all selective for Cs and therefore viewed as suited for these specific applications. Resins investigated were Gelwhite L, Clinoptilolite, Chabazite, Cabsorb (all inorganic) and Resorcinol formaldehyde (organic resin). Simliar data recently published by Zhang et al. for the resin ZMPP (zirconyl molybdopyrophosphate) was used as a bench mark to compare the recorded results with. Results of the Kd experiments (batch method, contact time is 24h) showed that at initial pH 1 to 4, the chabazite and clinoptilolite performed the best. At ph > 9, the RF resin and cabsorb had the higher Kd values, with Rf resin 7 times higher than chabazite. This correlate with literature results for the RF resin. The

16 April 25 – 29, 2005 5ICI

capacity experiments (batch method and column method) showed that the RF resin has the highest capacity for Cs. Reference: H. Y. Zhang, R. S. Wang, C. Sh. Lin and X. Y. Zhang; J. Radioanal. and Nucl. Chem., 247 (2001) 541 - 544. Track 1 – Session 9: Physical Measurements 52 Number theory of nuclide periodicity J.C.A. Boeyens University of Pretoria, South Africa The 81 non-radioactive stable elements occur in the form of 264 stable isotopes that separate into four modular series A(mod4)=0,1,2,3 with 81, 51, 81 and 51 members respectively. Each of these series can be further subdivided in terms of increasing neutron excess (A-2Z)(mod4), to yield 44 sequences, each of constant neutron excess (A-2Z)=0,43. These sequences are conveniently collated into 11 groups defined by A(mod24). Plots of experimental nuclidic binding energies as a function of either atomic or mass number also appear in the form of 44 linear segments that correspond exactly with the 44 linear number segments defined before. It follows, and it can be demonstrated that the 264 nuclides can be arranged into 11 sequential periods of 24 as a function of nuclear binding energy. The similarity between the scaled function of NBE(Z) and A(Z) is so striking that the observed periodicity can be formulated in terms of the integers A, Z and (A-Z) only. To highlight the effect of neutron excess on nuclidic stability the ratio Z/(A-Z) is plotted against Z, (A-Z) and A respectively. Each of these plots demonstrates a different aspect of the general periodic function. Of immediate importance is how the three plots demonstrate that the familiar periodic table of the elements, as well as the periodic structure inferred from the shell model of the nucleus, are subsets of the more general periodicity of the stable nuclides. Since both Z and (A-Z) are integers, the proton:neutron ratio for any nuclide corresponds to a rational fraction. Since rational fractions can be ordered into a complete set by the Farey sequence of number theory, the stable nuclides can be ordered by the same procedure. The resulting sequence of stable nuclides maps onto a well-defined sector of the Farey sequence. This sector is demarcated by the intersection of curves of constant neutron excess (A-2Z) with the rational fractions generated by the Fibonacci series that converges to the golden ratio of 0.6180... Using the well known properties of the golden ratio, simple formulae that define the beta-stability of all nuclides in terms of A, Z or (A-Z) are readily derived. The main conclusions that flow from the analysis are (i) self-similar relationship between nuclear and extranuclear structures; (ii) response of extranuclear structure to cosmic environment; (iii) logical definition of nuclear shell structure; (iv) mechanism of nuclear synthesis; and (v) prediction of cosmic abundances. These aspects to be discussed in more detail. 53 New developments in the production of Br-76 and I-124 B. Scholten, H.E. Hassan, S. Spellerberg, S.M. Qaim, H.H. Coenen Forschungszentrum Juelich, Institut für Nuklearchemie, Juelich, Germany The longer-lived positron emitters Br-76 (T½ = 16.0 h) and I-124 (T½ = 4.18 d) are attracting increasing attention for studying slow metabolic processes in man using the Positron Emission Tomography (PET). For production of Br-76, the Se-76(p,n) and As-75(3He,2n) reactions are commonly used. Regarding the Se-76(p,n)Br-76 reaction, the data base was weak. We recently completed a detailed cross section measurement in the low-energy range using highly enriched Se-76 targets. Furthermore, the chemical separation of radiobromine via thermochromatography was optimised. We also measured for the first time the excitation function of the reaction Kr-78(d,α)Br-76 from 5 to 13 MeV using highly enriched gas, however, demonstrating insufficient cross sections for production. For the production of I-124, four nuclear reactions, namely Te-124(p,n), Te-124(d,2n), Te-125(p,2n) and Te-126(p,3n), were

studied in low and intermediate energy regions using highly enriched isotopes. A comparison of all the processes was done. Targetry and chemical separation techniques have been well developed for the Te-124(p,n)I-124 reaction, which gives the pures 54 MNSR reactor power calibration with more than 3 MeV Gamma ray of reactor core M. Jalali1, J. Ebadati2, I. Shahabi2, M. Omidvar1, M. Mostajab Davati3 1Esfahan Nuclear Fuel Research & Production Center - Atomic Energy Organization of Iran, Nuclear Engineering Dept. Esfahan, Iran 2Esfahan Nuclear Fuel Research & Production Center, MNSR Reactor Department, Esfahan, Iran 3Physics Department, Esfahan University, Esfahan, Iran MNSR is an applied reactor with enriched fuel, light water moderator and Beryllium reflector with 30 KW maximum power and has been build basically for neutron activation analysis. Reactor neutrons react with core materials. The result of these reactions is delay and prompt gamma rays production in reactor environment. Reactor gamma spectrum in different powers and places has been measured with HPGe and NaI detectors. Gamma spectrum analysis resulted in the recognition, 235U (n, γ) 235U*, 9Be (n, γ) 9Be* and 27Al(n, γ)Al* reactions; which gamma energy of these reactions is more than 3 MeV dose not interfere with delay gamma energy. This project show that rate of prompt gamma production is directly to proportional reactor power. To have better data, reactor gamma spectrum more than 3 MeV energy has been used for reactor power calibration. 55 Method of charged-particle activation analysis M.A. Chaudhri1,2, M.N. Chaudhri1, Q. Jabbar3, Q. Nadeem3 1Pakistan Council of Scientific and Industrial Research, Laboratories-Complex-Lahore, Pakistan 2Institute of Medical Physics, Klinikum-Nuernberg, Nuernberg, Germany 3Physics Department, Lahore College University for Women, Lahore, Pakistan The accuracy of Chaudhri's method for charged-particle activation analysis 1, has been further demonstrated by extensive calculations. The nuclear reactions 12C(d,n) 13N, 63Cu(3He,p)65Zn, 107Ag(a,n) 110In and 208Pb(d,p)209Pb, whose cross sections were easily available have been examined for the detection of 12C, 63Cu, 107Ag and 208Pb respectively in matrices of Cu, Zr and Pb, at bombarding energies of 4 - 22 MeV. The "standard" is assumed to be in a carbon matrix. It has been clearly demonstrated that Chaudhri's method, which makes the charged particle activation analysis as simple as neutron activation analysis, provides results which are almost identical to, or only about 1-2 % different, from the results obtained by using the full "Activity Equation" involving solving complex integrals. It is valid even when the difference in the average atomic weights of matrices of the standard and the sample is large. Reference: 1. M. Anwar Chaudhri, G. Burns, E. Reen, J.L. Rouse and B.M. Spicer, J. Radioanal Chem, 37 (1977) 243. 56 Method of measuring of photochemical reaction quantum efficiency P.A. Bokhan, D.E. Zakrevsky, N.V. Fateev Institute of Semiconductor Physics, Siberian Branch, Russian Academy of Science, Novosibirsk, Russia Reactions of excited atoms with molecules can have an effective collision cross-section which considerably exceeds elastic one. These reactions are of practical interest for photochemical laser isotope separation. The most important parameter from this point of view is its quantum efficiency, which is a share of the excited atoms, reacted with a gas-reagent and forming a stable compound. This compound as the useful product can be easily extracted from the gas stream. The basis for the method is registration at the end of a stream the share of atoms reacted on the exposure to its laser

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radiation. The probability of a reaction of the excited atom with a molecule resulted from the exposure of to a single laser pulse is as follows: Θ=k1nτ0/1+(k1+k2)nτ0 (1) where k1, k2 are the rate constants of chemical and physical quenching of the excited state respectively, t0 is its natural lifetime, n is the gas-reagent concentration. After the exposure of M pulses the degree of removing of necessary isotope is defined by the expression: δ=1-(1-Θ·W)M (2) where W=s0Fβ/S is the atom excitation probability by a single laser pulse; s0 is the radiation absorption cross section; F is the photon flux per pulse; β is the share of atoms which interact with the radiation; S is the laser beam cross section. Measuring of the excited atom lifetime and using expressions (1,2) constants k1 and k2 and quantum efficiency η=k1n/(k1+k2)n+τ0

-1) are determined. Some results are demonstrated in the table. Reaction δ k1/k2 k1, 10-11,

cm3/s Rb(11P3/2)+(C2H5)2O RB(11P 3/2)+CH3OH Zn(4p 3P1)+(C2H5)2O Zn(4p 3P1)+H2

Zn(4p 3P1)+N2O Zn(4p3P1)+C2H5OH Zn(4p 3P1)+SF6 Zn(4p 3P1)+C3H12O

0.5 0.8 0.99 0.1 0.17 0.86 0.82 0.7

0.8 >10 0.25

4·10-3 6·10-3

0.1 0.2

6·10-2

40 150 30 0.1

8·10-3 0.1

5·10-2 8·10-2

57 Harmonisation of radioactivity measurements through SI-traceable primary standardisation and organisation of intercomparisons U. Wätjen, S. Pommé, T. Altzitzoglou, G. Sibbens, J. Keightley, R. Van Ammel, Z. Szántó EC-JRC-IRMM (Institute for Reference Materials and Measurements), Isotope Measurements Unit, Geel, Belgium The Radionuclide Metrology Sector of IRMM supports the international harmonisation of radioactivity measurements. It performs SI-traceable radioactivity measurements in the frame of primary standardisations, characterisation of reference materials, assessment of nuclear decay data, ultra-low level gamma-ray spectrometry and organises international comparisons of measurement among monitoring laboratories. IRMM has successfully participated in various so-called key comparisons of primary standardisation of radionuclide solutions. Work that is carried out to realise a common, SI-traceable measurement system, and which is performed in close collaboration with the International Bureau of Weights and Measures (BIPM), the Consultative Committee for Ionising Radiation (CCRI) and national measurement laboratories world-wide. Examples of recent primary standardisations, which do not rely on radioactivity calibration standards but purely on basic physical principles, are given. EU Member States are obliged under the EURATOM Treaty to monitor the levels of radioactivity in air, water and soil and to submit that information to the European Commission. IRMM applies its expertise in standardisation of radionuclides to address the comparability of measurement results by organising an annual comparison among the designated monitoring laboratories with reference samples. The method to establish reference values traceable to the SI units for such samples is discussed for the example of the first comparison exercise under this scheme, the γ-spectrometric determination of spiked 137Cs in air filters. Results of this comparison among 40 European laboratories are presented as well. Work of the group in the characterisation of matrix reference materials for their radionuclide content and applications in underground γ-spectrometry are described in separate presentations.

57a Isotope Transmutation for Radioactive Waste Minimisation M. Salvatores ANL-USA and FZK-Germany A sustainable development of Nuclear Energy requires that the issue of the management and minimisation of the radioactive wastes (arising from the irradiation of the nuclear fuel) is satisfactory solved. The need for a deep geological storage is well recognized for any sound strategy of waste management. However, in order to reduce the burden on it, the separation from the spent fuel of specific elements/isotopes and their successive transmutation into stable isotopes, has been explored by many leading laboratories since several decades, and encouraging results have been obtained, both theoretically and experimentally. Transmutation is achievable with neutron irradiation in a nuclear reactor and the related physics principles and processes will be recalled. Moreover, optimal strategies (reactor types and associated fuel cycles), will be described and justified. Finally, scenarios for their implementation will be shown, together with the programs underway to validate experimentally the concepts.

18 April 25 – 29, 2005 5ICI

Track 2 – Session 1: Labeled Compounds – Carbon Compounds 58 The synthesis of three isotopomers of LY354740, a potent and selective group II metabotropic glutamate receptor agonist W. Wheeler1, J. Monn2, M. Valli2, O'Bannon D.3 1Eli Lilly and Company, Toxicology & Drug Disposition, Indianapolis, IN, U.S.A. 2Eli Lilly and Company, Discovery Chrmistry, Indianapolis, IN, U.S.A. 3Eli Lilly and Copany, Isotopic Chemistry, Indianapolis, IN, U.S.A. As part of a program aimed at the design of conformationally constrained analogs of glutamic acid, LY354740((+)-2-aminobicyclo[3.1.0]hexane-2,6-carboxylic acid) was identified as a highly potent, selective, group II metabotrophic glutamate receptor agonist. The C-14 labeled isotopomer of LY354740 was synthesized and used extensively in pre-clinical ADME studies. Tritiated LY354740 was synthesized as well for use in receptor binding assays. Later in the development of LY354740, a stable labeled isotopomer of the racemic modification of LY354740 was synthesized for use as an internal standard for LC-MS-MS assays. In this poster, the preparation of these isotopically labeled compounds will be discussed. 59 The synthesis of C-14 labeled LY379268 and LY389795 , potent and selective group II metabotropic glutamate receptor agonists W. Wheeler1, M. Spence2, F. Kuo2 1Eli Lilly and company, toxicology and drug disposition, Indianapolis, IN, USA 2Eli Lilly and Company, Isotopic Chemistry, Indianapolis, IN, USA Recent efforts have identified agents that are highly potent, selective, and systemically active group II metabotropic glutamate receptors. Heterocyclic analogs of LY354740 have been synthesized in which the C-4 methylene has been replaced by an oxygen atom (LY379268) and a sulfur atom (LY389795). C-14 labeled isotopomers of these compounds have been synthesized to facilitate pre-clinical ADME studies. A stable labeled isotopomer of LY389795 (as a racemic mixture of LY389795 and its enantiomer) has been prepared for use as an internal standard for bioanalytical assays. In this poster, the preparation of these isotopically labeled compounds will be discussed. 60 Clinical measurements of carbon-14 labeled compounds using accelerator mass spectrometry (AMS) B. Keck Procter and Gamble Pharmaceuticals, Analytical Sciences, Mason, Ohio, USA Accelerator Mass Spectrometry (AMS) was originally developed for the purpose of carbon dating. The measurement relies upon the use of carbon-14 as a rare stable isotope, rather than radioactivity decay. Sensitivity can be significantly superior to conventional liquid scintillation counting (LSC). We have been applying this methodology to present biomedical AMS results in a conventional manner. Topics discussed include: the carbon isotope pools, direct AMS versus HPLC-AMS, the fundamental differences between AMS and LSC, and the limits of quantitation for direct AMS. In a biomedical AMS experiment, there are three isotopically distinct sources of carbon: the labeled compound, the biosphere pool of carbon and the petrochemical carbon. However, if a separation is employed, as in HPLC-AMS, the goal is to greatly reduce the biosphere carbon and add petrochemical carbon as carrier. In direct AMS, an aliquot of sample is dried into a quartz vial, where it is catalytically oxidized to carbon dioxide and reduced to graphite and placed in the source of the spectrometer. With HPLC-AMS, chromatographic separation is employed prior to graphite preparation, increasing complexity. For physical methods in pharmaceutical science, it is often considered acceptable to have an uncertainty of 15 percent or less expressed as a coefficient of

variation. This includes the compounded uncertainties of both the carbon concentration and isotope ratio for direct AMS, and all factors involved in the case of HPLC-AMS. These issues have been examined in the context of a clinical study to measure the long term concentration of two different compounds. Potential clinical patients were screened, isotope ratios in varying geographies were measured, effects of sample collection procedures were identified and limits of quantitation were established in urine and serum. All patients screened were found to be normal with regard to radiocarbon. Sample collection procedures play a small but relevant role in determining the limits of quantitation. The direct method of AMS resulted in meeting the sensitivity, precision and accuracy goals; extending the assay sensitivity by three orders of magnitude beyond LSC. 61 Deuterolabelling of butyrolactone type dietary lignan metabolites M. Pohjoispää, E. Leppälä, K. Wähälä University of Helsinki, Department of Chemistry, Laboratory of Organic Che, Helsinki, Finland Lignans are widely distributed plant natural products with diverse biological activity. The metabolism of some plant lignans has been studied both in vivo and in vitro and they have been shown to convert to the mammalian lignans enterolactone and enterodiol in intestines. Recently number of new plant lignan metabolites have been identified. The growing interest in these compounds is based on their possible health effects and further on quantitation of these compounds in biological samples. Quantitation of lignans requires good resolution and sensitivity because lignan concentrations are quite low in human fluids. The analytical techniques used for lignans are based in HPLC-MS or GC-MS1. In these methods stable isotopic labelled lignans are needed as internal standards to quantitate enterolignans in man. We have developed a deuterium labelling method but butyrolactone type lignans using D3PO4 · BF3 complex prepared in situ2. This method exchanges all aromatic protons to deuteriums giving stable deuterolabelled compounds in good yield and high isotopic purity3. 1Hoikkala, A.A.; Schiavoni, E.; Wähälä, K. Br. J. Nutr. 2003, 89, Suppl. 1, 5-18. 2Wähälä, K., Rasku, S. Tetrahedron Lett., 1997, 38, 7287-7290. 3Leppälä, E., Wähälä, K. J. Label. Compd. Radiopharm., 2004, 47, 25-30. 62 Synthesis of carbon-14 analogue of 1,5 diaryl-5-[14C]-1,2,3-triazoline and triazoles H. Matloubi, N. Saemian, G. Shirvani, F. Johari Daha Nuclear Research Center (ABOI) , Chemical Division, Tehran, Iran 1,5 diaryl-1,2,3-triazoline and triazoles frequently exhibit anti-convulsant properties and compare favorably with prototype antiepileptic drugs1. The presence of the methylsulphone group at the para-position of one of the phenyl rings in analogues compounds, has let to compounds with good anti-inflammatory properties2 and cyclo-oxyganase enzyme inhibitor potency3. To further elucidate the mechanism of action and to support the on-going metabolism studies4 the need arose to synthesize the corresponding carbon-14 compounds, with the label situated in a biologically stable site5,6. The desired products, were synthesized according to the synthetic pathway shown in following Scheme7,8.

Ba14CO3 K14CN Cu14CN X I

X 14CNX 14CO

HNH2H3CO2S

14CN

XSO2CH3

H N

NN

14C

X SO2CH3Triazoline

N

NN

14C

X SO2CH3Triazole

a b

c

d

e

f

g

5ICI April 25 – 29, 2005 19

X=H, -CH3, -OCH3 a) K, KN3. b) CuSO4, Na2S2O5. c) DMF. d) Raney-Ni, HCO2H. e) EtOH/THF. f) CH2N2, Dioxane. g) KMnO4, n-Bu4N+Cl-, Benzene, H2O. 1Kadaba, P.K., J. Med. Chem. 1988: 31, 196 2Li, J.J., Nortone, M.B. et al. J. Med. Chem. 1996: 39, 1846 3Talley, J.J., et al. J. Med. Chem. 2000: 43, 775 4Sunay, U.B., et al. J. Labelled Compd. Radiopharm. 1992: 31, 1041 5Matloubi, H., Saemian, N. et al. Appl. Radiat. Isot. 2002: 57, 501 6Matloubi, H., Shirvani, G. et al. J. Labelled Compd. Radiopharm. 2002: 45, 347 7Matloubi, H., Saemian, N., Shirvani, G., Johari, F., Appl. Radiat. Isot. 2004: 60: 665 8Matloubi, H., Saemian, N., Shirvani, G., Johari, F., J. Labelled Compd. Radiopharm. 2004: 47, 31. 63 Modified synthesis of 8-Chloro-11-(4-methyl-1-piperazinyl)-5H-dibezo(b,e)(1,4) diazepine-11[14C] and its derivatives N. Saemian, H. Matloubi, G. Shirvani Nuclear Research Center / AEOI, Chemical Division, Tehran, Iran Tricyclic rings systems possessing a dibenzo structure joined to a central seven -membered heterocyclic ring with a basic side chain have been a rich source of biologically active molecular entities and frequently show effects on the central nervous system [1]. During the last 30 years, a number of antipsychotic agents belonging to the chemical class of dibenzo epins have been introduced (i.e. Clozapine, Loxapine, Clothiapine and other analogues of these compounds). The precise mechanism of action of these compounds are not known [2].Therefore to further elucidate the mechanism of action and to support ongoing metabolism studies,there arose a need for analogues of these compounds carbon-14 labelled in a biologically stable site. In this report, Ba14CO3 was converted to K14CN using Potassium azide by heat treatment[3]. Cu14CN was preapared from K14CN in presence of CuSO4 and sodium metabisulfite[4]. In the next step, 2- amino - benzo - nitrile [cyano-14C] was derived from a addition of Cu14CN to 2- iodo - benzamine. The latter product was coupled with 1,4- dichloro - 2 - nitro benzene in hot DMSO. Then, the resulted nitrile was hydrolysed to amide with basic hydrogen peroxide in DMSO[5]. The reduction of nitro group and cyclization were accomplished in one step in the presence stannous chloride in acetic acid as the reducing agent and the key lactam 8-chloro-5,10-dihydro - 11H - dibenzo [1,4][b,e] diazapine -11-one -11 [14C] was produced in good yield[6]. The key lactam was converted to 8-Chloro-11-(4-methyl-1-piperazinyl)-5H-dibezo[b,e][1,4] diazepine -11 [14C], in a one pot operation by reaction with the complex of N-methyl piperazine and titanium tetra chloride[7]. In the next step synthesis of analoge of 8-Chloro-11-(4-methyl-1-piperazinyl)-5H-dibezo[b,e][1,4] diazepine -11 [14C] with chemical structure, 8-Chloro-11-(4-methyl-1-piperazinyl) dibez[b,f][1,4] oxazepine -11 [14C] was carried out. In this approach 2- hydroxyl benzo nitrile [cyano-14C] was drived from the addition of K14CN and CuI to 2- iodo phenol using potassium salt of 2- hydroxyl benzo nitrile [cyano-14C] instead of 2- amino benzo nitrile [cyano-14C] in synthetic path way of 8-Chloro-11-(4-methyl-1-piperazinyl)-5H-dibezo[b,e][1,4] diazepine -11 [14C], a successful synthesis of 8-Chloro-11-(4-methyl-1-piperazinyl) dibez[b,f][1,4] oxazepine -11 [14C] was achieved[8].

Ba14CO3 K14CN Cu14CNa b

I

YH YH

14CN

+

Cl

Cl

NO2 Y

14CN

NO2

Cl

Y

14C

NO2

Cl

O

NH2

Y

NH14CCl

O

Y

N14CCl

NMP

c d

e

fg

a) K, KN3 b) CuSO4.5H2O, Na2S2O5 {Y:NH: c) Cu14CN d) Cs2CO3, DMSO e) K2CO3, H2O2, DMSO} { Y: O: c) CuI, K14CN d) KOH, DMSO e) Cs2CO3, H2O2, DMSO} f) SnCl2, AcOH, EtOH g) TiCl4, NMP References [1]. Steiner, G., Franke, A., Hadicke, E., Lenke, D., Teschendorf, H.J., Hofmann, H.p., Kreiskott, H., Worstmann, W., J.Med.Chem. 1986; 29: 1877 [2]. Klunder, J.M., Hargraue, K.D., West, M.A.,Cullen, E., Pal, K., Behnek, M.L., Kapadia, S.R., Macneil, D.W., Wu, J.C., Chow, G.C., Adams, J., J.Med.Chem. 1992; 35: 1887 [3]. Perry, C.W., Burger, W., Dlaney, C.M., J.Labelled Cpd. Radiopharm. 1978; 16; 645 [4]. Manning, C.O., Wadsworth, A.H., Fellows, I., J.Labelled Cpd. Radiopharm. 2002; 45: 611 [5]. Katritzky, A.R., Pilariski, B., Urogdi, L., Synthesis.1989; I: 949 [6]. Matloubi, H., Saemian, N., et al., Applied Radiation & Isotopes. 2001; 55:789 [7]. Chakrabarti, J.K., et al., J.Med.Chem. 1989; 32: 2375 [8]. Matloubi, H., Saemian, N., et al., Applied Radiation & Isotopes. 2002; 57: 501 Track 2 – Session 2: Labeled Compounds – Hydrogen Compounds 64 Tritide reagents for the synthesis of tritiated natural C compounds H. Andres Isotope Laboratory Novartis Pharma AG, Basel, Switzerland Early pharmacological and pharmacokinetic studies of highly potent natural compounds usually require the use of radiolabelled isotopomers. Since carbon-14 labelling normally involves low-yielding multi-step syntheses and gives insufficient specific activity for binding studies tritiation is preferred. Standard labelling methods such as catalytic tritiation often fail for macrocyclic natural compounds and polyketides because of double bonds and other reducible groups. For this reason a series of tritide reagents had to be developed which exhibit high functional selectivity. Starting from lithium tritide, sodium tritide, or sodium borotritide, tri-butyltin tritide, lithium tri sec-butylborotritide, sodium triethylborotritide or tetramethyl-ammonium tris-acetoxyborotritide were prepared. Natural compounds such as Rapamycin, Sanglifehrin, Discoder-molide and others could be labeled with high incorporation of tritium. 65 Expedient incorporation of Tritium into drug candidate C. Berthelette, J. Scheigetz, C. Li, R. Zamboni Merck Frosst Canada, Medicinal Chemistry, Montreal, Quebec, Canada In the course of our medicinal chemistry efforts, we have discovered a series of compounds with good affinity for the prostaglandin D2 (PGD2) receptor and thus required further metabolism and protein covalent binding studies best carried out by incubations with radiolabeled compounds. A common feature present in several of these compounds was a methyl aryl sulfone or a methyl aryl ketone moiety. Tritium labeling of the methyl groups by exchange carried out on the final compounds seemed an easy alternative to a total synthesis approach. Herein, we wish to report a fast and efficient base-catalyzed exchange reaction to deuterate and subsequently tritiate the methyl group of our drug candidates. Deuterium incorporation ranging from 46 to 99% was calculated using mass spectrometry and the results from these exchanges were used as guidelines for tritium labeling giving specific activities in the range of 28 to 120 mCi/mmol (1.03 GBq/mmol to 4.43 GBq/mmol). In comparison, tritium labeled 2,3,4,9-tetrahydro-1H-carbazoles were also prepared in good yields with specific activities ranging from 4.2 to 7.0 Ci/mmol (155-214 GBq/mmol) when subjected to catalytic tritium-bromine exchanges of the corresponding aryl bromide precursors. These 6-bromocarbazole precursors can only be made via a multi-step synthesis. Our current base-catalyzed exchange reaction represents an attractive method for the rapid introduction of tritium in one step for various compounds possessing a methyl aryl sulfones or ketones.

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66 The synthesis and use of Tritium-labeled drugs in clinical studies at Abbott Laboratories G. Rotert1, N. McCracken1, D. Hickman1, B. Surber1, T. Pagano1, J. Darbyshire1, M. Emery1, S. Swanson1, T. Stratton1, I.Yu. Nagaev2, V.P. Shevchenko2, N.F. Myasoedov2, A.B. Susan3 1Abbott Laboratories, USA 2Institute of Molecular Genetics, Russian Academy of Sciences, Russia 3International Isotope Clearing House, Inc., Leawood, KS, USA Tritium-labeled drugs are rarely used in clinical studies because of "classical/old fashioned" concerns about the possibility of the formation of so-called "labile tritium". We have found that if the appropriate choices are made with respect to the position of the tritium label(s) and preliminary animal ADME studies show little loss of tritium, tritium-labeled drugs were very useful alternatives to 14C-labeled ones. We have synthesized and then successfully used a number of these in clinical studies. The results from one of them, [3H]ABT-358 were part of the NDA submission that lead to the marketed product, Zemplar. The main reason for using tritium labeled drugs in this study was the problem posed by the very low dose that had to be given for the compound requiring high-specific activity (needed to detect and measure their metabolites) that was obtainable with 3H but not 14C. For another study, we synthesized [2,11,31-3H]ABT-578 from [2,11,31-3H]rapamycin, which was made by I.I.C.H.***Inc./I.M.G.**, via a proprietary isotope exchange method. The use of [2,11,31-3H]ABT-578 made from [2,11,31-3H]rapamycin in ADME studies was the only reasonable alternative since the products made by other labeling methods either resulted in the loss of the label or called for prohibitively high costs. The excellent results obtained in the clinical study using the product made from [2,11,31-3H]rapamycin will be part of the Abbott NDA submission for our proprietary drug-eluting stent device. The details of the challenges presented by the syntheses of the above compounds and the overall results of the studies are described. 67 Tritium labelling of novel endomorphin analogues containing unnatural alpha- and beta-amino acids T. Geza1, E. Szemenyei1, A. Keresztes1, F. Fülöp2 1Biological Research Center of Hungarian Academy of Sciences, Institute of Biochemistry, Szeged, Hungary 2University of Szeged, Institute of Pharmaceutical Chemistry, Szeged, Hungary New endomorphin-2 analogues containing 2',6'-dimethyl-tyrosine (Dmt) and/or alicyclic-beta-amino acids ((1S,2R)-2-amino-cyclopentane carboxylic acid (Acpc) and (1S,2R) 2-aminocyclohexane carboxylic acid (Achc)) were designed and synthesized (Tóth, G., Keresztes, A., Tömböly, Cs., et al. Pure Appl.Chem.76 (2004) 951)) to obtain more active and more selective mu- and delta-opioid receptor ligands with higher stabitity against proteolytic enzymes. The most promising analogues (Dmt-Pro-Phe-Phe-NH2, Tyr-(1S,2R)Acpc-Phe-Phe-NH2 and Tyr-(1S,2R) Achc-Phe-Phe-NH2) were labelled with tritium. First, we synthesized precursor peptides (3',5'I2Dmt-Pro-Phe-Phe-NH2, Dmt-Delta-Pro-Phe-Phe-NH2, Tyr-Delta(1S,2R)Acpc-Phe-Phe NH2 and Tyr-Delta(1S,2R)Achc-Phe-Phe-NH2) by SPPS method. The dehydro-beta-amino acids and their Boc-protected derivatives were synthesized in racemic forms by literature procedure (Fülöp, F. Chem.Rev.101 (2001) 2181)). The diastereomeric peptides were separated by HPLC. The configuration of the dehydro-beta-amino acids in the peptides was determined by chiral TLC using enantiomeric standards. The appropriate precursor peptide isomer was used for the tritium labelling. The tritium labels were introduced in the different amino acids by saturation of the double bond in the peptides containing dehydro-proline or dehydro-beta-amino acids or dehalogenation of the peptide containing diiodo-dimethyl-tyrosine using tritium gas and Pd/BaSO4 catalyst. The crude tritiated peptides were purified by radioactive HPLC. The specific radioactivities of the final products were 1-1.6 TBq/mmol. The novel labelled peptides have become useful tools for the opioid research in our laboratory. Supported by OTKA T046514

Track 2 – Session 3: Labeled Compounds – Other Compounds 68 Investigation of the influence of metallic impurities on the Y-90 labelling yield of dota-tate D. Pawlak1, R. Mikolajczak1, J.L. Parus1, A. Korsak2, I. Sasinowska2 1Radioisotope Centre POLATOM, Research and Development, Otwock, Poland 2Radioisotope Centre POLATOM, Analytical Laboratory, Otwock, Poland Introduction: DOTA-conjugated peptides labelled with radionuclides such as Y-90 or Lu-177 can be used for peptide receptor radionuclide therapy (PRRT), however high specific activity of both radionuclides and radiolabelled preparation are required. DOTA derivatives form thermodynamically stable complexes with Y but some cations are strong competitors for them. The influence of these cations, considered as contaminants, on the labelling yield of DOTA-peptides was systematically investigated. Several potential sources of metallic contaminants: the radioisotope solution, compounds used for labelling, vials and stoppers, reagents were considered. Aim: Our study was undertaken in order to evaluate influence of metallic impurities on radiochemical purity of Y-90 labelled DOTA-peptides. The investigated carrier-free radionuclide Y-90 was produced at the Radioisotope Centre POLATOM. Methods: DOTA-TATE was labelled according to the published methods. To the labelling vial a volume of 50 µl of 0,4 M sodium acetate containing 40mg/ml of ascorbic acid and 6 mg/ml dihydroxybenzoic acid (pH=4,5) was added followed by 25 µl of DOTA-TATE (10 µg or 100 µg) in 0,4 M acetic buffer (pH 4,5) and varying quantities of Y-90 to give molar ratio of chelate to radiometal from 4:1 to 75:1. The concentration of each analyte (Fe, Cu, Zn) was verified by ICP-Optical Emission Spectrometry. The labelling yields were determined by HPLC and/or SepPak separation. Results: The investigation confirmed that the presence of metals such as Fe, Cu, Zn significantly decreases the Y-90 labelling yield of DOTA-TATE. When the molar ratio of Fe to peptide was < 0.4 the labelling yields were > 95%. In case of Zn and Cu similar yields were achieved when metal to peptide molar ratios were < 0.6. Conclusion: Chemical purity of Y-90 is crucial for efficient labelling of peptides planned for use in PRRT. 69 A comparison of high and low specific activity Lutetium-177 for radiolabeling peptides and proteins C. Bensimon1, S. Oelsner2, P. Danks1, A. Chan1, H.R. Maecke2, S. Good2 1MDS Nordion, Nuclear Medicine, Kanata, Canada 2University Hospital, Radiological Chemistry, Basel, Switzerland Aim: Lutetium-177 (Lu-177) is of interest in developing new targeted radiotherapies because of its low energy beta, non-volatile nature, radiological half life and ability to be imaged. Some peptides and proteins, like Substance-P and Bombesin display pharmacological side effects. Therefore only very small quantities of these peptides can be administered to patients, limiting the side effects due to the peptide or protein. The aim of this research is to provide evidence that high specific activity Lu-177, when compared to low specific activity Lu-177, is more effective in the development of formulations with increased activity per fixed amount of chelate-peptide conjugate. This is particularly useful for developing drug products with pharmacologically active peptides and proteins. Method: High specific activity product derived from Yb-176 and low specific activity derived from Lu-176 were evaluated. Labeling conditions were optimized at room temperature and/or 40°C to achieve the lowest molar ratio chelate/Lu-177 using DOTA and DTPA with the shortest reaction times and highest yields achievable. Using these labeling conditions, high and low specific activity Lu-177 were compared using DOTA and DTPA with and without conjugates.

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Results: Using a reaction time of 1 hour and reaction temperatures of 40°C or room temperature, DOTA and DTPA conjugates were radiolabeled with yields of greater than 95%. The molar ratio of Lu-177 /chelate was found to be 2 to 3 times greater with high specific activity Lu-177 compared to low specific activity isotope. High specific activity Lu-177 permitted higher amounts of activity to be chelated to a minimum quantity of conjugate. Conclusion: High specific activity Lu-177 with a very low impurity profile permits radiolabeling of chelated peptides and proteins at room temperature or 40°C to achieve high specific activities (mCi/mg of protein). High specific activity Lu-177 provides the advantage of increasing the amount of activity that can be labeled to a limited amount of conjugate, thus facilitating the development of new targeted radiotherapeutic peptides and proteins where pharmacological activity may be a concern. 70 The preparation of 99mTc-Zoledronate S.N. Luo1,2, H.Y. Wang1,2, M.H. Xie1, Y.J. He1, X.Y. Liu2 1Jiangsu Institute of Nuclear Medicine, Wuxi, China 2Southern Yangtze University, Wuxi, China Zoledronic acid [2-(imidazol-1-yl)-hydroxy-ethane-1,1-diphos-phonic acid],has been approved for the treatment of multiple myeloma and for patients with bone metastases from solid tumors. In order to explore 99mTc labelled zoledronic acid (99mTc-zoledronate) as imaging agent for bone metastases, 99mTc-Zoledronate was prepared by the reduction of Na99mTcO4 with SnCl2 in aqueous solution. The effects of SnCl2, pH, zoledronic acid, Na99mTcO4 and temperature of reaction to the labelling yields of 99mTc-Zoledronate were studied. The results showed that when pH was between 3-7, the mounts of SnCl2 and zoledronic acid were over 20µg and 2.0mg respectively, and at room temperature the reaction continues above five minutes, the radiochemical purity of 99mTc-Zoledronate determined by TLC of bis-system was over 95%. 99mTc-Zoledronate was stable for 24 hours. Initial results of biodistribution in mice showed 99mTc-Zoledronate was a potential bone imaging agent. 71 Preparation of [64Cu]pyruvaldehyde-bis(N4-methylthio-semi-carbazone) Complex as a PET and/or therapeutic Radio-phar-maceutical A.R. Jalilian, P. Rowshanfarzad, J. Moafian, M. Kamali-dehghan, M. Mirzaii, M. Sadethi, H. Noorkojoori, H. Bakhtiari Cyclotron & Nuclear Medicine Department, Nuclear Research Center for Agriculture and Medicine (NRCAM), Atomic Energy Organization of Iran, Karaj, Iran Cupper-64 (T½=12.7 h) is an important radionuclide used both in PET imaging and therapy. [64Cu]-pyruvaldehyde-bis(N4-methyl-thiosemicarbazone) ([64Cu]-PTSM) is one of the most famous copper radiopharmaceuticals with unique specifications (suitable half life, stability etc.). The wide range of 64Cu applications arouse great interest for its production. Cu-64 was produced via the 68Zn (p,αn) 64Cu) nuclear reaction and isolated from the irradiated target by a two-step chemical method. [64Cu]-PTSM was prepared using in-house made PTSM ligand and [64Cu] cuprous acetate. The complex formation parameters (time, temperature, concentration and elution methods) were determined carefully. Copper-64 was prepared in chrloride form (≈200 mCi, >95% chemical yield at 180 µA for 1.1 h irradiation, radionuclidic purity >96%, copper-67 as impurity). The solution of 64Cu-PTSM was prepared in >80% radiochemical yield and more than 98% radiochemical purity. Quality controls and stability tests were performed for the final solution. [64Cu]-PTSM was prepared at the radiopharmaceutical scales with high quality and has a potential for use in therapeutic/imaging centers.

72 Comparison of the preparation and quality of 131I-MIBG produced with fission and activated 131I M. Letsoalo1, O. Knoesen2, D.J. Niemann2 1NECSA, NTP Radioisotopes, Pretoria, Gauteng, South Africa 2NECSA, Radiochemistry, Pretoria, South Africa Introduction: Iodine-131 is the most widely used iodine isotope. Meta-Iodobenzylguanidine (mIBG), labelled with 131I, has extensive use in nuclear medicine to localize and treat neuroendocrine tumours such as pheochromocytomas and neuroblastomas. NTP Radioisotopes has been the supplier of diagnostic and therapeutic 131I-mIBG for the past 20 years in South Africa. Up until 2000, 131I-mIBG has been labelled with activated 131I whereafter fission 131I was used. The labelling procedures are different but the results are reproducible with radiochemical purities of ≥ 95%. The quality of 131I-mIBG from two different labelling processes and sources of 131I is compared. The variable parameters such as volume, temperature and time are different for the two processes, yet optimum values for both are obtained. Up to 700mCi of 131I should be able to bind to the mIBG. The radiochemical purity must be greater than 95% to meet the minimum product specifications. Materials and method: Labelling with activated 131I Weighed masses of mIBG and CuSO4 were dissolved in 0.2N H2SO4 on a water bath at 60 ºC. 131I was added and the solution heated in an autoclave for 30 minutes. After heating, the 131I-mIBG compound was eluted through an anion exchange column. The pH was adjusted to pH 4.2 and the solution filtered through a 0.22 µm filter. 1% Benzyl alcohol solution was added as a preservative to the dispensed product. Labelling with fission 131I CuSO4 was dissolved in 0.2N H2SO4, added to the mIBG powder and heated on a water bath at 60 ºC until dissolved. 131I was added and the solution heated at 175 ºC for 45 minutes. The pH was adjusted to 4.2, the solution eluted through an anion exchange column and filtered through a 0.22 µm filter. 1% Benzyl alcohol in water was added as a preservative to the dispensed product. Quality Control of the 131I-mIBG Each production batch was analysed by ascending paper chromatography (Whatman No.1) with 2:1 methanol: demineralised water as the mobile phase. Results and discussion: Five consecutive runs were performed with radiochemical purities above 95% from both processes. Table 1: Results from the 131I-mIBG prepared from activated and fission 131I

Activated 131I Batch 153MT 154MT 155MT 156MT 157MT RC% 95.74 98.74 96.12 95.74 98.17

Fission 131I Batch 233MT 234MT 235MT 236MT 237MT RC% 96.17 97.40 97.17 95.70 96.28 Conclusion: The above procedures yield radiochemical purity above 95% and NTP's 131I-mIBG has been used around South Africa with good clinical results and no side effects reported. 73 Radiosynthesis and preliminary evaluation of 131I-dota-tate as a potential tracer for somatostatin receptors visualization V. Lungu1, D. Niculae1, D. Chiper1, P. Albert2 1Natl Inst for Physics and Nuclear Engineering, Radiopharmaceuticals, Bucharest, Romania 2Institute of Oncology, Nuclear Medicine, Bucharest, Romania The purposes of this work were to study, select and optimize the radiosynthesis parameters of 131I-DOTA-TATE and to determine the specific biological properties asked for an imaging agent. The electrophilic radioiodination of DOTA-TATE, using chloramines-T (Cl-T), leads to good radiochemical purities (95.2% - 95.8%) in the following conditions: DOTA-TATE to 131I molar ratio: 1.7; DOTA-TATE to Cl-T molar ratio: 0.09; pH: 7.4, 0.01M PBS; gentisic acid as stabilizer. The 131I-DOTA-TATE was stable 6 days at 4-8 °C. The competition binding assay and the saturation binding assay of 131I-DOTA-TATE were performed using rat brain cortex membrane

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as biological somatostatin receptor model. The pharmacological parameters values IC50 = 1.28 nM and Kd = 157.6 pM recommend this radiopeptide as potential agent for somatostatin receptor tumor imaging. Track 3 – Session 1: Dating , Soil and Water 74 Applicability of environmental radionuclides in soil. What is known from depth profiles of 40K, 226Ra, 210Pb and 137Cs in temperate and tropical forest soils? R. Fujiyoshi, T. Paces, R. Zimmermann, K. Sakamoto, M. Shibata, M. Suzuki, Y. Suzuki, T. Sumiyoshi, S. Sawamura Depth profiles of environmental radionuclides (40K, 226Ra, 210Pb and 137Cs) were investigated in temperate and tropical forest soils to trace underground environmental changes including biological activities. The sites focused in this study were located in Germany (Wetzstein, Tharandt, Hainich and Leinefelde), in Czech Republic (Lysina, Pluhuv Bor and Nacetin) and in Peru (Alto Mayo) as well as at several points on the campus of Hokkaido University, Sapporo, Japan. Predominant stands in Europe were described to be coniferous in Germany (Wetzstein and Tharandt) and also in Czech Republic (Lysina, Pluhuv Bor and Nacetin), deciduous in Germany (Hainich and Leinefelde) and mixed in Japan with various stand age classes. In Peru, there are typically two types of forests, i.e., tropical tall rain forests and low heath forests. Many of the sites have been affected anthropogenically like acid precipitation, fall-out of radionuclides by atomic bomb tests or accidents of atomic power plants, and burning field. Hydrological and geochemical monitoring of the environment has been continued in those places. Soil samples were carefully collected by hand at individual sites from 2001 to 2004. After drying and homogenizing, a part of each sample was used for getting data on soil properties (humidity, organic content, soil pH and CEC). Gamma spectrometry with two types of HPGe detectors was applied to obtain activity concentration of each nuclide of interest. Depth profiles of 40K activity concentrations in soil generally reflected mineral composition of the soil to increase its activity with soil depth. However, there appeared minimum and maximum values at several soil depths under coniferous forests in Germany. It may be due to either soil homogeneity or underground biological activities like root uptake and movements of smuggling bioorganisms. Such a bioturbation could be evaluated by considering all the profiles of individual nuclides obtained at a site of interest. For example, patterns of anthropogenic 137Cs and a part of 210Pb profiles could suggest how extensively and intensively the soil would have been disturbed. Both nuclides generally show surface enrichment in natural and semi-natural soil environment. The results obtained at each site will be discussed along with data on soil properties and hydrological data. It is concluded that the environmental nuclides of different chemical properties and of different origins would be quite useful for estimating possible changes occurring or having been occurred in soil environment 75 Environmental isotopes and hydrochemical study for groundwater exploration and development in the Afar Depression, Northeastern Ethiopia A. Tenalem, K. Seifu, A. Tamiru Department of Geology and Geophysics, Addis Ababa University, Addis Ababa, Ethiopia Environmental isotopes (2H and 18O, tritium, few 13C and 14C) and hydroichemical study was carried out to assess the hydrogeological system of the vast drought prone Afar Depression, which is one of the dries and hottest places on earth. The aim is to explore and develop the scarce groundwater resources. The isotope and hydrochemical analysis is supported by conventional field hydrogeological survey. The region is tectonically active volcanic terrain bordered by rift escarpment and highlands having large topographic differences ranging in elevation form -120 below sea

level to around 4,000 masl. Rare surface water bodies characterize the region; often seasonal ponds formed by flush floods and highly alkaline lakes with only one perennial river (Awash) draining the vast desert. The study revealed that recent meteoric water is the major source of recharge. Three distinct groundwater zones were identified associated with the highlands, transitional escarpment and the rift. Towards the rift the ionic concentration and isotopic enrichment (2H and 18O) increases following the groundwater flow paths, which is strongly controlled by the axial rift faults. The groundwater converges to the seismically active volcano-tectonic depressions with internal drainage (in places occupied by terminal lakes) and to the Awash river. Within the Afar Depression at least four groundwater regimen are identified: 1) fresh and shallow groundwater associated with alluvial deposits ultimately recharged by isotopically depleted recent highland rainfall and the Awash river, 2) cold and relatively younger groundwater within localized fractured volcanics showing mixed origin, 2) old groundwater with extremely high ionic concentration and low isotopic signature localized in deep fractures and, 4) Old and hot saline groundwaters connected with geothermal systems. The study clearly demonstrated that dependable groundwater can only be obtained from the first two types in aerial restricted zones in flat plains following river courses, local wadies and volcano-tectonic depressions. Generally this integrated study enabled to understand the surface water-groundwater interactions and helped in developing the conceptual hydrogeological model of the region under data (aquifer test and well head observations) scarce conditions. 76 Nitrate in South African ground water resources: isotopes suggest natural production of high levels and a feasible supply solution B.Th. Verhagen1, M.J. Butler2, E. van Wyk3 1University of the Witwatersrand, School of Geosciences, Johannesburg, South Africa 2Tirisano of Ithemba LABS, Johannesburg, South Africa 3Department of Water Affairs, Division of Geohydrology, Pretoria, South Africa High nitrate concentrations - sometimes in excess of 100 mg L-1 NO3-N- are endemic Limpopo Province of South Africa, to a large extent dependent on ground water. High nitrate poses a considerable health risk, such as intestinal cancer in adults & methaemoglobinaemia in infants. Thusfar, attention has been focussed on potential anthropogenic sources such as agriculture and sewage disposal. However, a recent joint environmental isotope, hydrochemical and geohydrological study on ground water resources, suggests that important natural processes could also be responsible. The area of study is underlain by the Carboniferous to Tertiary Karoo sedimentary sequence of sandstones and siltstones, which is capped by basalt. Except for fracture zones associated with a fault, the relatively shallow ground water levels stand in the basalt. Ground water development was therefore to a large extent restricted to the relatively shallow basalt aquifer. Modelling radiocarbon and tritium data suggests an uncoupling of these two isotopes used traditionally for estimatign ground water residence times. Thermonuclear 14C appears to move more rapidly to the saturated zone than 3H. These points to deep-seated root systems of phreatophytes endemic in the area, such as acacia erioloba, amongst others. Such roots can transport significant amounts of biogenic CO2 into the saturated zone of the basalt aquifer at or below the water table, resulting i.a. in renewed and ongoing chemical weathering & precipitation processes within the saturated zone, usually completed in soil and vadose zone processes. Correlations with other solutes such as silica and carbon-13 in TDIC are further indicators of the weathering process. Roots produce CO2 not only by respiration but also through the decay of the functional (fine) roots, seasonally discarded from the structural root systems. Anaerobic bacterial decay processes liberate nitrogenous nutrients, which in turn can be mineralised to NO3. Nitrogen isotope studies support these conclusions. As a natural process, deep-seated nitrate production is not readily mitigated for

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supply purposes. Prompted by the results of these studies, further exploration revealed an extensive and deeper sandstone aquifer, with high yields of good quality, renewable ground water. Conjunctive use of the two aquifers, with isotope & hydrochemical monitoring, could lead to resource quality management strategies. 77 Determination of Cl and Ca concentration in Zayandeh Roud River with PGNAA method M. Mostajab Davati1, M. Jalali2, K.H. Rezaee1 1Esfahan University, Physics Department, Esfahan, Iran 2Esfahan Nuclear Fuel Research & Production Center, Atomic Energy Organization of Iran, Nuclear Engineering, Esfahan, Iran Cl and Ca concentrations in water of Zayandeh Roud river have been measured with PGNAA technique in suburban of historical Esfahan city (Iran). Experiment has been done with HPGe detector and Cf-252 neutron source in PGNAA lab in Research & Production fuel center (Esfahan). With standard solutions of CaCO3 and NaCl in experiments, the values of average Cl and Ca concentrations have been determined to be 75.7 ppm and 86.4 ppm respectively. 78 Labelling of humic substances with 14C and their use for sorption studies with different geomatrices A. Mansel, H. Kupsch Institute of Interdisciplinary Isotope Research, Georadiochemistry, Leipzig, Germany The reactive carbon compounds (humic substances, HS) of the dissolved organic matter (DOC) dominate the spreading of inorganic and organic pollutants in the biogeosphere. The classical analytical methods such as TOC-detection and UV-spectroscopy are of limited use in the lower concentration range (< 1mg/l), usually found in environmental samples. By using radiolabelled HS, scenarios near to nature in the µg/l-HS-concentration range can be studied. Based on our promising results of the HS radiolabelling with 14C diazonium ions, we applied these radiolabelled substances first time to sorption studies under conditions, usually found in subterranean waste repositories. The natural HS (humic acid HA, fulvic acid FA) were purified by the IHSS-procedure. Aldrich-HA (AHA), Gorleben-HA (GoHy-532), an adequate HA (HS3), a terrestrial HA (HS4), a lignite HA (HAL) and an aquatic FA (FS3) were used for our investigations. A synthetic HA (M42) was provided by the Forschungszentrum Rossendorf. The radiolabelled HS were contacted in aqueous solution with a sandy soil, granite, diabase and kaolinite in batch experiments under conditions near to nature. Adsorption isotherms of various radiolabelled humic acids were determined depending on geomatrix, pH, HS concentration, contact time and heavy metal content. The behaviour of the radiolabelled HS was not influenced by the labelling procedure. With the use of radiolabelled humic substances a concentration range below mg/l can be studied. 79 Characterisation of reference materials for radioactivity: the example of milk powder and soil intercomparison materials T. Altzitzoglou, M. Bickel, A. Bohnstedt, J.G. Decaillon, C. Hill, L. Holmes, G. Sibbens EC JRC – IRMM (Institute for Reference Materials and Measurements), Isotope Measurements Unit, Geel, Belgium Food or environmental matrix reference materials characterised for their radioactivity contents are very important as they are used to calibrate measurement instruments and validate analytical methods. The Institute for Reference Materials and Measurements (IRMM) participated in an IAEA co-ordinated research project by characterizing two reference materials, namely milk powder and soil. Radioactivity levels in milk and soil are of particular concern since milk is an important component of human nutrition, especially for children and soil is a natural matrix important in environmental monitoring. The activity concentration of actinides, 226Ra and 90Sr was assayed in the given materials. The analysis was first done non-destructively by low-level γ-ray spectrometry. Then,

a radiochemical procedure based on microwave digestion or leaching and followed by extraction chromatography was developed to isolate the actinides, Ra and Sr from the matrices. The activity of the actinides and 226Ra were measured by alpha-particle spectrometry and that of 90Sr by ultra low-level liquid scintillation counting. This article gives an overview of the procedure followed, including the chemical separation and the measurement methods employed. Since traceability of the results to the SI units is essential for certified reference materials, the traceability issue is described briefly. 80 Underground gamma-ray spectrometry – a new tool to look for isotopic fingerprints M. Hult, J. Gasparro, U. Wätjen EC-JRC-IRMM, (Institute for Reference Materials and Measurements), Isotope Measurements, Geel, Belgium Cosmic rays are responsible for a large part of the background in gamma-ray spectrometry. A great reduction (up to 4 orders of magnitude) of the background count rate can be achieved in gamma-ray spectrometry by performing it deep underground. Underground gamma spectrometry opens the field for isotopic fingerprints. By this we mean the capacity to detect certain radionuclides that are present in extremely small quantities but are indicative of a certain process. With interference free detection limits in the order of 1 mBq it is possible to detect fewer than 1000 atoms of radionuclides with half lives in the order of 10 to 100 days. For long lived radionuclides such as Al-26 (72,000 years) the interference free detection limits are higher (around 1010 atoms, which corresponds to some pg in mass) but still low in comparison with many other techniques. In recent years the field of underground gamma-ray spectrometry has developed from being solely an instrument in fundamental physics to being used in fields such as environmental studies and industrial applications as well as an alternative to more laborious techniques such as radiochemistry under specific condition. This presentation will deal with the state-of-the art as well as giving examples on new applications. Track 3 – Session 2: Atmosphere, Space and Environmental Monitoring 81 Risk of transfer of some actinides in the form of volatile oxides and hydroxides in the atmosphere V.P. Domanov Joint Institute for Nuclear Research, Dubna, Moscow, Russia Formation of volatile oxides of nat.U, 237Np, 238,239Pu and 241,243Am was observed. They were produced under thermal oxidation of trace quantities of these actinides in a stream of the He and O2 mixture. The volatile compounds were separated by the thermochromatographic (TC) method. The initial sample was purified quartz powder with actinides in question adsorbed on the surface of SiO2-particleas. It was placed into the starting zone of an empty quartz TC column. The results of the experiments showed that the uranium compounds were transported along the column and adsorbed at 450±25°C, 250±25°C and 120±25°C. The deposition zones were found with an α-spectrometer. Volatile neptunium compounds were adsorbed in two zones with the centers at 475°C and at 300°C. The location of the plutonium deposition zones resembled the distribution of the uranium adsorption zones; besides one more very volatile compound deposited at a negative temperature about -100°C was registered. An increase in the efficiency of uranium and plutonium transport into the third zone (120±25C°) with the enhancement of the gas humidity can be connected with formation of volatile hydroxides. Americium formed only two adsorption zones located at 400-450°C and 200-250°C. For the interpretation of the results obtained, model experiments with trace quantities of 249Cf and carrier-free 185Os, 183Re, 97Ru and 96Tc radioisotopes were performed. It was shown that 249Cf formed volatile dioxide adsorbed at 450±25°C. It was also found that other model radioisotopes in a stream of helium with a negligible touch of oxygen were adsorbed at 450-500°C and 250-300°C in the forms of dioxides and trioxides, respectively.

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Based on these data, it is assumed that the first adsorption zone (400-500°C) appears due to formation of actinides dioxides and the second one (200-300°C) appears due to formation of trioxides. Comparison of the 185OsO4 and 97RuO4 adsorption zones with the fourth adsorption zone of plutonium (-105±25°C) indicates their similarity. We can draw a conclusion that octovalent plutonium was produced, which in a form of very volatile PuO4 deposits at a negative temperature. The results obtained point to the possibility of migration of oxidation products of uranium, neptunium, plutonium and americium in the atmosphere after nuclear tests and accidents at nuclear power plants. It was concluded that dioxides and trioxides of actinides can migrate in the atmosphere by an aerosol mechanism, the volatile tetraoxide PuO4 can be transferred by airflow and the transfer of volatile U and Pu hydroxides can be affected by a mixed mechanism. 82 Studying the effects of 1974 French Atomic Tests series in the Pacific on Australian Atmosphere - An activation analysis approach to nuclear metrology M.A.Chaudhri, M.N.Chaudhri1,2 1Pakistan Council of Scientific and Industrial Research, Laboratories Complex, Lahore, Pakistan 2Institute of Medical Physics, Klinikum Nürnberg, Nürnberg, Germany Principle: A novel apprach for nuclear metrology has been selected to study the effects of French Atomic Tests in the Pacific of 1974, on the Australian atmosphere. This is to investigate the changes in the elemental concentrations of the atmospheric particulates collected in Australia just before and after the onst of the atomic tests in the Pacific. Any additional radioactivity due to the tests would either be still there or would decay into stable isotopes. If by some very sensitive techniques one could determine the elemental/isotopic composition of the air particulate, one can work backwards in estimating the sort and quantity of activities that could have ecisted just after conducting of the tests. We decided to use the technique of charge-particled activation analysis to estimate the elemental/isotopic concentrations of the Australian Atmosphere. This technique has the potential to provide concentrations in the ppb and sub ppb regions. Method: the atmospheric particulates were collected on Polystyrene filters in high-volume air samplers placed all along the Australian East Coast at locations in Port Moresby (New Guinea), Townsville, Brisbane, Sydney, Melbourne and Hobart. The filters were cut into small pieces and placed in the grove of an A1-Target holder, covered by a thin A1-foil, which was cooled by liquid nitrogen. The samples were irradiated for one hour each with a proton beam of 8.5 MeV at an intensity of 1 µA. After a waiting period of one hour the irradiated samples were counted with a high resolution and high sensitivity Germanium detector. Suitably prepared "Standards" for quantifying the absolute concentrations, were also irradiated in identical fashion and their induced activities measured. Results and discussion: a number of elements, S, Ca, Ti, Cr, Fe, Ni, Cu, Zn, Se and Hg were detected in the two types of samples - one taken just before the Atomic Tests started and the other set taken just after the finishing of the tests. Their concentration of different elements ranged from 0.001-3.27 µg/m3. Certain changes in the concentrations of different elements were observed in the two sets. However, these changes were attributed to synoptic effects rather than due to Nuclear Fall-out Effects. The ease, strenght and potential of this sort of approach for nuclear metrology would be discussed. 83 Isotope dilution and isotope mixture calculations in support of the Gallium solar neutrino observatory experiment M. Wallenius, S. Millet, K. Mayer, K. Lützenkirchen European Commission, Joint Research Centre, Institute for Transuranium Elements, Karlsruhe, Germany In the Gallium Neutrino Observatory (GNO) experiment solar neutrinos are studied. These low energy neutrinos interact with 71Ga and produce radioactive 71Ge via an inverse electron capture

reaction in gallium, 71Ga(νe,e) 71Ge. This germanium isotope decays with a half-life of 11.43 days and its decay is used for quantifying the number of solar neutrinos observed. Stable Ge isotopes are used as carriers when some ten atoms of 71Ge are extracted from a 100-ton of gallium chloride target after a month's exposure time. The carrier serves at the same time to quantify the chemical yield of the extraction process. An unavoidable phenomenon of the extraction process is that some of the Ge carrier remains in the Ga-tank and it is desorbed only during the following extraction(s). Applying different enriched Ge isotopes (70Ge, 72Ge, 74Ge and 76Ge) in alternating sequence allows identifying incomplete extraction of the carrier by high precision isotope ratio measurements. These are carried out using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). The exact quantification of any residual Ge carrier from the preceding run is achieved through isotope dilution calculations. Isotope dilution mass spectrometry is basically a two component approach (usually quoted as "spike" and "sample") and normally makes use of two isotopes, i.e. a single ratio. In our evaluation we noted that using different ratios for the IDMS calculation lead to inconsistent results. We therefore applied a multi-component approach, making use of all the isotope ratios. The algorithms are the same as applied for synthetic isotope mixture calculations. In this paper we describe the evaluation of the results using the two-isotopes and two- components approach, as well as multi-isotope and three components approach. The benefits of the three component approach will be described in detail. For the GNO experiments we could show that the measured isotopic composition of the carrier after extraction can be fully modelled by a mixture of the initially used Ge carrier, of the Ge carrier from the previous run and of a small, but non-negligible contribution of natural Ge. 84 Radiological continuous monitoring of the environment: beyond the scope of the nuclear industry P. Van Put, A. Debauche, J.-P. Lacroix, C. De Lellis National Institute for Radioelements (IRE) , Fleurus, Belgium The very first nuclear metrology tools for surface water radiological surveillance have been designed in the early 80's. From their rudimentary characteristics, they have evolved nowadays to a stage reducing considerably the gap between the performance level of laboratory analysis and analysis performed continuously in the environment. Technical evolutions in the fields of computer sciences (embedded operating system, low power consumption microprocessor) and telecommunication (GSM, satellite) mainly have allowed the IRE to develop an original instrument able to detect and to quantify very small radioactivity increase in surface water. This system is based on a gamma spectrometry analysis of the medium and it is featured by a very good sensitivity, a low false detection rate, a very good stability and limited maintenance. As an example, the sensitivity achieved in seawater for the most common isotopes is less than 10Bq/m³ in a radiation background at least 1000 times higher. The design of the detection system without sampling equipment make feasible to feed it with solar energy. Until not long ago, the main goal of this tool was to detect the accidental releases of nuclear installations (power station, reprocessing plant, radioisotopes production). One concrete example is the HYDROTELERAY (supplied by IRE) measurement stations network that monitors continuously the radioactivity level of the French rivers for the benefit of the IRSN. Following the pressures from different organisations and with the "zero-release" policy in mind, other industries are at present concerned by the continuous surveillance of the effluents generated by their activities. Among different sectors, lets mention the hospitals and the industries generating NORM material (phosphate, gypsum, ...). As an illustration, this presentation will feature the very first data acquired in a water purification plant collecting sewage water from hospitals. In another context, lets mention also the psychological importance that represents this control in the sector of drinking water and in the sector of fish farms that use warm water directly supplied from a nuclear power plant third loop. The interest of these systems is also demonstrated following incidents involving nuclear driven submarines in the Mediterranean sea and the threats of malignity acts by natural resources radiological contamination

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("dirty bombs"). These thoughts are expressed through an IRE project starting in the Mediterranean Sea and by implementation studies in the Middle East. Finally, such an instrument finds also some uses in research applications as in the fields of pollutants dispersion modeling, hydrogeology, oil prospecting, ... 85 Curium-244 alpha sources for space research V.M. Radchenko, M.A. Ryabinin, L.S. Lebedeva Federal State Unitary Enterprise State Scientific Centre, Research Institute of Atomic Reactors, Russia Total requirements for alpha-sources used in alpha-proton-X-ray spectrometers (APXS) for space objects analysis are presented in the report. Methods for preparation of active core of unsealed alpha-sources are discussed, e.g. electrodeposition of radioactive material on combined substrates followed by reductive annealing, and curium-244 oxide metal thermal reduction followed by metal curium vapor condensation on various substrates. The sources have been shown to keep their spectral parameters both after mechanical (impact, vibration) and thermal-vacuum (from - 196 up to + 1000 centigrade) test. Application of sources for the Mars rock analysis during the Mars Pathfinder (in 1997), Spirit and Opportunity (in 2003) NASA missions is described in the report. 86 Short-time variations of cosmogenic 7Be concentration in near-surface air of the town of Como (Italy) M. Pellicciari, E. Andreotti, A. Giuliani, M. Pedretti Universita dell'Insubria, Dipartimento di Fisica e Matematica, Como, Italy 7Be is a gamma-emitting cosmogenic radionuclide very useful as a tracer for atmospheric circulation, as an indicator of stratospheric intrusion and as a test of mathematical model for transport and dispersion of pollutions. Both pollutions and meteo-parameters have variations on a short-time scale (i.e. hours). Therefore, in order to better understand possible correlations, short time collection of 7Be are necessary. Since 7Be atmospheric concentrations are of the order of a few mBq/m3, very good gamma-ray sensitivity is required to study daily variations. An underground station (rock cover is about 300 m water equivalent) for the measurement of low level radioactivity is in operation in Northern Italy in the town of Como under the Baradello hill (Laboratorio Sotterraneo del Baradello), where a 30% HPGe detector with a radio-pure copper shielding has been installed. Our sensitivity to 7Be in the Laboratorio Sotterraneo del Baradello is better than 1 mBq/m3. This allows us to collect and analyse this nuclide for short time intervals. We have carried out therefore a campaign of measurements aiming at characterizing the atmospheric variability of 7Be concentration in short temporal intervals (11.5 h) and to find possible correlations with atmospheric parameters and pollutions. The campaign has taken place as follows: - we have collected samples of atmospheric particulate on paper filters for temporal intervals of about 11.5 h (i.e. one measurement during the day and one during the night) at the 7th floor of the main building of Universita' dell'Insubria in Como; - after collection, we have analyzed the filters with the HPGe installed in the Laboratorio Sotterraneo del Baradello, in order to estimate the activity of 7Be through gamma spectrometry; - the concentration of 7Be in air was determined from the gamma activity of the filters; - we have studied the variations of 7Be concentration and looked for correlations with meteo and pollution data. In particular we have found a strong correlation with temperature, a good correlation with O3 and a remarkable anti-correlation with SO2. Simple qualitative considerations allow to understand these trends. The particularity of such a campaign is to have performed measurements relevant for atmosphere physics exploiting low level gamma ray spectrometry.

Track 4 – Session 1: Tracers 87 Boron injection neutron life logging technology and its applications in oilfield development P. Zhao PetroChina Company Limited, Beijing, China This paper introduces the theory of Boron Injection Life Logging technology and its application examples in Huabei, Jidong, Dagang and other oilfields in China. The applications illustrate that this technology provides a feasible and effective logging method for oilfield watered out zone evaluation and residual oil potential tapping. 88 Positron emission particle tracking and other applications of the Birmingham LC40 Cyclotron D. Parker, X. Fan, A. Ingram, M.D. Smith University of Birmingham, School of Physics and Astronomy, Edgbaston, Birmingham, UK Apart from its major role in medicine, Positron Emission Tomography (PET) can also be used to study industrial processes. For over 20 years the University of Birmingham has been using positron-emitting tracers to study a wide range of systems drawn from engineering and the physical sciences. To complement conventional PET imaging, the technique of positron emission particle tracking (PEPT) was developed, whereby a single labelled tracer particle can be tracked at high speed inside operating equipment. PEPT has been used to study a variety of phenomena involved in the flow and processing of granular materials, and more recently to study the flow of viscous fluids by means of neutrally-buoyant tracer particles. Since early 2004 the radioisotopes for this work have been produced using a Scanditronix MC40 cyclotron, which was purchased second-hand from the VA Medical Center, Mineeapolis in 2002 and installed at Birmingham during 2003. Radioisotopes including 18F and 61Cu are used to label single particles down to 100micrometres in diameter. The cyclotron is also being used for other isotope production, surface activation and radiation damage studies. 89 Use of activated nanoparticles as a tracer for an additive to diesel fuel F. Tondeur1, I. Gerardy1, J. Guillaume1, L. Rocher2 1Institut Supérieur Industriel de Bruxelles, Nuclear Unit, Brussels, Belgium 2Rhodia Electronics and Catalysis, la Rochelle, France Eolys, a fuel-borne catalyst made by Rhodia to regenerate filters for Diesel particulate abatement (DPF), is composed of nanoparticles of Ce/Fe oxides. Besides its performances as a catalyst, one has to control its retention by the DPF to avoid a dissemination of residues. Filtration efficiencies >99% were obtained for Ce by a VERT test [1], not conclusive for Fe, due to the impossibility to separate Fe coming from the engine and from Eolys. Isotopic methods might provide a solution. We use radioactive Ce and Fe as tracers of Eolys. Neutron activation is used to introduce radioactive Ce/Fe in Eolys particles. Activation is usually not seen as a good way to label a compound, due to the modifications induced by the Szilard-Chalmers effect, but the recoil energy responsible for this effect should not produce strong alterations to the nanoparticles. The measurements are done by gamma spectrometry. The emission of 141Ce(146 keV) does not interfere with the lines of 59Fe(>1 MeV). The sample is activated at SCK-CEN. The tests are done at ISIB with a Citroën C15 Diesel engine and a C5 DPF. The exhaust gas is sampled with controlled flow before and after the DPF. Soot and particles are collected on a multi-layer inox textile. The sampling efficiency is evaluated by extrapolating the activities measured on the successive layers. The tests include (a)tests during standard cycles (b)comparison between low regime

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(no regeneration) and high regime (higher temperature for regeneration). The results of the study are: (a) All measurements show the same Fe/Ce ratio, indicating that Fe from Eolys behaves like Ce, so conclusions obtained for Ce in [1] can be extended to the Fe of the additive. (b) The efficiency of the DPF is better than 99,9 % for Eolys particles, confirming the VERT test. (c) There is no indication of a stronger release during regeneration. (d) A part of the activity is trapped in the motor and/or the exhaust pipe before reaching the DPF, only roughly evaluated in our study (appr. 80%). It is released with delay. To which extent Ce/Fe particles may accumulate, and their release may evolve in the long term, is not examined here. Our results are valid for an engine without prior use of Eolys and a new particle trap. We thank the BR1 group at SCK-CEN for their support with neutron activation. [1] EMPA test report 420'150, Swiss Federal Laboratories for Material Testing and Research, 2001 (confidential). 90 Reproductive performance of cows by using isotope M.A.S. Khan Department of Dairy Science, Bangladesh Agricultural University, Mymensingh, Bangladesh Indigenous cows were studied to find out the reproductive constraints under village condition of Bangladesh by using 125I. Sixty seven postpartum cows were taken from 65 small holder farmers. Selected animals were used for dairy/ draught purpose. Cows were rice straw based diet. Calves were allowed to free access for suckling cows during day and were tied up at night. Nutritional Metabolic Kits supplied by the Food and Agriculture Organization of the United Nations/ International Atomic Energy Agency (FAO/IAEA) were used for metabolic profile study and the FAO/IAEA Progesterone Radioimmunoassay (RIA) kits were used for progesterone (P4) measurement by using 125I as tracer. A relatively high concentration of P4 at a given time indicates the presence of an active corpus luteum in the ovaries, while the basal concentration indicates its absence. Calving to first ovulation was calculated on the basis of basal concentration of P4 in milk. Reproductive events were measured. Data were analyzed by 4 seasons to find out the reproductive constraints of indigenous cows. The plasma urea values (mmol/ L) of cows were 4.5, 7.2, 5.5, and 3.2 for the seasons Summer, Autumn, Winter and Spring respectively. The calving to first ovulation were 66, 67, 187 and 51 days; to first service were 272, 120, 191 and 216 days; to first conception were 283, 136, 197 and 223 days; and calving interval were 544, 419, 489 and 501 days for the seasons Summer, Autumn, Winter and Spring respectively. Among the blood metabolites studied, a considerable change in urea values were noticed. It represents a nutritional constraint on reproduction. The spring values were lower enough to suggest a shortage of Rumen Degradable Protein (RDP) in the ration. The calving to first service was higher than that of calving to first ovulation, that means farmers were unable to detect heat of their cows. So, heat detection was a constraint to the reproduction of indigenous cows. The calving to first service in the Autumn was shorter than that in the other 3 seasons. It would be tempting to relate to the urea levels that were highest in the Autumn. From this study two important constraints of reproduction has been identified for the indigenous cows where interventions are needed; (1) Nutritional constraints in general, mainly protein, during the Spring season and (2) Lack of knowledge of estrus detection by the farmers during the early part of lactation which decrease the reproductive efficiency of cows.

Track 4 – Session 2: Nucleonic inspection and radiation applications 91 Reconstruction of 60Co radiation image based on charge successive integration Z. Wu, X. Guo INET, Tsinghua University, Beijing, P.R. China In the scan radiography system, there are many ways to measure and sample the output signals from image detector array. A new method, named periodically successive integration of electric charge from detector cell, is put forward and realized to acquire image data in this paper. That means to take a certain time slice Tm as the integral period, successively measure the total electric charge output from the detector cell during each period Tm by integration. And each measurement value is sampled and digitized to be one image pixel value. This mode is quite different from the conventional sample mode. All the detector output information associated with the inspected object is collected. And it can be applied not only to the continuous signal, e.g. the detector output from radiography system with the radioactive isotope source, but also to the pulse signal, e.g. the detector output from imaging system with linear accelerator source. Generally speaking, the measuring period (i.e. integral period) Tm is equal to the sampling period Ts because each measurement value acts as one sample value (i.e. image pixel value). However, Ts would be determined by the requirement of image spatial resolution, while Tm is limited by some hardware conditions such as process circuit response time, data transfer time and so forth, thus Tm and Ts may be different sometimes, which will lead to degradation of image quality or geometry distortion. In order to solve this problem, in this paper, an equivalent physical model is set up to emulate the radiation measurement system based on periodically successive integration of the detector output electric charge, and the corresponding mathematical expressions are given out. And the image data reconstruction theory and algorithm are hereby developed. All those are well employed in TC-SCAN Co-60 train cargo online radiography inspection system, and the system performance is greatly enhanced. The maximum train velocity matching the TC-SCAN system is improved from 15km/h to 45km/h. insert images a) Actual image acquired at a velocity of 22.5km/h

b) corresponding image reconstructed

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92 Cobalt-60 container CT inspection system J. An, H. Wu, J. Liu, L. Wang, P. Cong INET (Institute of Nuclear Energy Technology), Tsinghua University, Beijing, China To determine the material of goods inside container (or truck) is very important for the fight against terrorism. The current container scanners, no matter which kind of radiation source is used, cannot fulfill this task. Because these are based on the digital radiography technique (DR), and the images obtained are just only projection images. The goods at front or back position are overlapped on the projection image, and the gray scale is depended on the total mass thickness along the rays. We suggested a new way to solve this problem - applying CT Technology to inspect container, pallet, car or other large objects. The sample machine of 60Co container CT (fig.1) had been constructed in 2003 and has been working well now. The 60Co source is of 100 Ci. The conveyor system can push the object be scanned at the speed of 18m/min to get the projection image. The big ring can roll around container at the speed of 2 revolution/min to get the section image. Fig.2 and fig.3 show the projection images of a car at horizontal and perpendicular direction. Fig.4 shows its section image at front wheel. Fig.5 shows the section image of an air-cargo. There are three bottles inside it. Gasoline is in the left bottle, water is in the middle bottle, and in the right bottle are half water and half gasoline. Because the density of gasoline and water is different, the responding gray scale is different and can be separated easily on the section image. Using pseudo color to show gray scale, the difference between gasoline and the water is very distinct, as shown at the left corner of fig5. A piece of soap, which is hidden inside a box of grease, can also be found out. According to fig.2~5, it is proved that the container CT system posses the performance of getting projection image at different direction and getting section image at different position of large object and can determine material quality by the gray scale on the section image. These performances are very useful not only for the fight against terrorism but also for anti-smuggling. Fig. 1.1

Fig. 1.2

Fig. 2

Fig. 3

Fig. 4

Fig. 5

93 Design and realization of a radiometric Gauge intended for control on line of the coatings of galvanization on sheet steel R. Alami1, R. Cherkaoui2, K. Laraki1, H. Ghazlane1, A. Charif1, S. Mimount1, L. El Badri1, A. Benahmed1 1CNESTEN, B.P. 1382 R.P. 10001 Rabat 2LPNR, Faculté des Sciences Rabat, B.P. 1014, Rabat The steel plates produced by the Maghreb-Steel company are covered with a layer of Zinc in order to increase their corrosion resistance. To control continuously the thickness of the Zinc layer, which is about 30 to 45 mm, Maghreb-Steel company contacted the CNESTEN in order to develop a device based on the x-ray

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fluorescence technics (Source: Am 241 300 mCi, Detector: CaF2), to allow this control depth except for the percent/ This project (gauge KALFAN (of Arabic Kalfana: galvanisation)), consists of: O/ sensors (Source: Am 241 300 mCi, Detector: CaF2) O/ Data acquisition System O/ Positioning System and Mechanical stand. This gauge (KALFAN), designed for realt ime adn uninterrupted control, of the coating of galvanisation of steel plates, was installed on the line of galvanisation of the Maghreb-Steel company and functions since under normal conditions. 94 Radiation grafting of styrene onto PFA film for the development of a proton exchange membrane (PEM) for a fuel cell P.H. Kang, Y.C. Nho, K.R. Park Koreo Atomic Energy Research Institute, Radiation Application Division, Daejon, Korea PFA (poly(tetrafluoroethylene-perfluoropropylvinylether) grafted polystyrene sulfonic acid (PFA-g-PSSA) membranes were prepared by simultaneous irradiation method, using gamma-radiation from a 60Co source at room temperature in air. The absorbed dose and dose rate ranged from 50-200 kGy and 10kGy/h, respectively. The effect of grafting conditions such as the types of diluent solvent, the irradiation dose and dose rate, as well as the styrene concentration in the grafting solution on the degree of grafting was investigated. The pysico-chemical properties of the PFA-g-PSSA membranes such as the degree of grafting (DOG), ion exchange capacity (IEC), water uptake and tensile strength were evaluated. The structure variations after grafting and sulfonation were investigated using FTIR-ATR. Thermogravimetric analysis (TGA) has been used to study the thermal decomposition of the grafted PFA films. The mambrane electrode assemblies (MEA) based on PFA-g-PSSA membrane bonded carbon supported catalyst; platinium for the anode and cathode were prepared. The MEAs were evaluated with a fuel cell system and a single cell test rig with 4 x 4 cm active area by using hydrogen as a fuel. The results showed that the degree of grafting was strongly dependent upon the dose rate and the type of solvent as well as the styrene concentration. The irradiation dose was also important grafting condition to mechanical strength of the grafted membrane. Some of the grafted membranes have a considerably lower resistance and higher power density than the most widely used membrane Nafion. The radiation-grafting technique is considered as one of the processes to synthesize the proton-exchange membrane (PEMs) for a fuel cell. 95 Enhanced mutants of pendimethalin degrading bacterium, Bacillus sp. ms202 induced by gamma radiation H.-Y. Chung, Y.-K. Lee, H.-H. Chang, Y.-S. Jang Korea Atomic Energy Research Institute, Radiation Application Research Division, Yuseong, Daejeon, South Korea To induce the enhanced mutants of dinitroaniline herbicide pendimethalin degrading bacterium, Bacillus sp. MS202 was irradiated by gamma radiation at the dose of LD95(3 kGy). Enhanced mutants (MS202m7, MS202m14, MS202m18) were isolated morphologically using clear zones formed around their colonies on plates contained pendimethalin(1,000mg/l). From GC analysis, the degrading activity of each enhanced mutant(MS202m7, MS202m14, MS202m18), the formation of pendimethalin metabolite, increased 11.0%, 45.1%, and 31.6% than the control, respectively. It suggested that mutant induction by gamma radiation could be a useful tool for the enhancement of pesticide degradation by microbes. 96 The role of prussian blue in eliminating the compositional effects of 137Cs internal contamination A.E. Fekry1, Elwan K.M.1, S.M. Mangood2 1Nuclear Research Center, Egyptian Atomic Energy Au, Biological Applications Department , Cairo, Egypt 2Nuclear Research Center, Egyptian Atomic Energy Au, Radiation Protection Department, Cairo, Egypt

70 male albino rats of two ages: growing (2-months age, 102 g /rat) and adults (4- months age, 280 g / rat) were used in this study. The rats were fed on a balanced diet (21% crude proteins, 3% crude fats and 4% crude fibers). The treatments of oral administration of a single dose (3700 Bq/growing rat and 7400 Bq/adult rat) of 137Cs (137Cs Cl salt) and prussian blue (PB, 300 mg/kg body weight/day for 60 days) were as the following combinations: [1] without 137Cs or PB, [2] 137Cs only, [3] PB only, [4] PB one day before 137Cs, [5] PB immediately after 137Cs, [6] PB one day after 137Cs, and [7] PB one week after 137Cs. All of body weight, total body water (TBW), fat-free body (FFB), total body fat (TBF), fat-free dry body (FFDB), total body protein (TBP), and total body ash (TBA). The data revealed that: adult rats had a significant (P>0.01) more mean values of final body weight, TBW, FFB, TBF, FFDB, TBP, TBA than growing rats. In both of growing and adult rats, 137Cs treatment caused decreases in final body weight; % change of body weight, TBW, FFB, FFDB, TBP, TBA. In both growing and adult rats, PB administration, only before or at the same time of irradiation, could eliminate the effects of 137Cs-gamma irradiation on: final body weight, % change in body weight, FFB, FFDB, TBP. However, PB administration, one or seven days post 137Cs, eliminated 137Cs treatment's effects on TBF Track 5 – Session 1a: Medical Isotope Applications I 97 Glucose tolerance, body composition and degenerative diseases in elderly people living in Quemado de Guines, Cuba M. Hernandez-Triana1, G. Sanchez-Alvarez2, V. Ruiz-Alvarez2, S. Gonzalez-Calderin1, M. De la Paz-Luna1, M.E. Diaz1, G. Salazar-Rodriguez2 1Institute of Nutrition, Bichemistry and Physiology, Havana, Cuba 2Institute of Nutrition, Stable Isotopes Lab, Santiago de Chile, Chile Overweight (42%), hypertension (33.5%) and diabetes (3.6%) are high prevalent in the Cuban population. Subjects with abnormal glucose metabolism have at least one or more of the other cardiovascular disease risk components which classified in the Metabolic Cardiovascular Syndrome. Insulin resistance and glucose intolerance have been proposed as common etiological factors of this syndrome; physical inactivity and low total energy expenditure should also have a determinant influence. Its prevalence in active rural elderly subjects living in a mountain community of the island was however 19%. With the purpose to study the frequency of the syndrome and its relations with other cardiovascular disease risk components, a study was carried out in 216 urban elderly subjects living in central Cuba. Body fatness was assessed by anthropometry and electrical bioimpedance. The deuterium dilution method was used as reference standard of body composition. Biochemical indicators of glucose and lipids metabolism and Helicobacter pylori antibodies were accompanied by a 3d dietary recall, physical activity by questionnaires, clinical and epidemiological examinations. Only very few individuals were at dietary risk of energy and macronutrients deficiency. On the contrary energy from total and animal fat was consumed in levels of 42% and 68% by the subjects. Overweight affected 21% of men and 50% of the women. Obesity was 8 times higher in women. Increased abdominal fat accummulation affected 20% of men and 52% of women. Fat accummulation in the whole body measured by skinfold thickness averaged from 1.4 to 2.2 times the fatness estimated by BMI or waist circumference. Body fat measured by deuterium dilution, 33% of women and 19.6% of men, was more coincident with skinfold thickness than bioimpedance. The 25% of the subjects with abnormal levels of serum glucose had a significantly higher prevalence of obesity, abdominal fat, hypertension, inactivity, hypertriglyceridaemia, hypercho-lesterolaemia, and raised LDL values. The prevalence of the Metabolic Cardiovascular Syndrome aroused values of 18%. The elderly subjects of that community were classified as carriers of a cluster of risk factors which, alone or in a synergistic way, contribute to the major death causes in the island at the moment.

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98 Preparation of 99mTC-Hynic-Annexin V and its biologic evaluation for in vivo imaging apoptosis D. Chen1,2, X. Jin1, B. Qi1, Z. Luo1, B. Jia1,2, H. Yang1, H. Cui1, J. Zhang1, J. Du1, D. Ma3, F. Wang1,2 1China Institute of Atomic Energy, BAHT, Beijing, China 2Medical Isotope Research Center, Peking University, Beijing, China 3Human Disease Genomic Research Center, Peking University, Beijing, China Apoptosis is an intimate component of normal organ function, which keeps the whole body balance. The process of programmed cell death, or apoptosis, has been one of the most intensively studied topics in the biological sciences during the last 3 decades. One of the important characteristics of the early apoptosis is the exteriorization of phosphotidy lserine (PS). Annexin V has high affinity for PS exposed on the cell membrane, which become the important marker of detection of early apoptosis. The in vivo imaging research of radiolabeled Annexin V have made great progress in recent years, which would have been improving the comprehension about disease, prediction of response to disease therapy and development of new drugs so on. In current study, Annexin V was derivatized with Hydrazinonicotinamide (HYNIC) and coupled to Technetium 99m(99mTc) before i.v administration in animal models of apoptosis. HYNIC, a nicotinic acide analog, is a bifunctional molecule capable of bonding to lysine residues of proteins on one moiety and conjugates of 99mTc on the other. The agent forms stable complexes with proteins without affecting bioactivity. The domestic recombinant human Annexin V have been radiolabeled with 99mTc and the feasibility of in vivo imaging apoptosis with the labeled compounds have been evaluated. Besides the synthesis of Succinimidyl 6-HYNIC (S-HYNIC) and linking of S-HYNIC with Annexin V, the preparation of 99mTc-HYNIC-Annexin V had been finished, while the analytical methods of TLC and HPLC had been established. (1) S-HYNIC had been synthesized and characterized by IR, 1H-NMR and elemental analysis. The three key problems (DMF remove, anhydrous condition and BOC remove) had been solved during the synthetic process. (2) Coupling conditions: 1mol Annexin V (5.5mg/mL) was derivatized with 6mol S-HYNIC in 20mmol/L HEPES for 5hr shielded from light, one Annexin V coupled two HYNIC. The coupling conditions of Annexin V concentration and reacting solvent had been systematically investigated. 99 Development of new brachytherapy seeds based on Tm-170 G. Shani1, A. Hwaree1, I. Orion2 1Ben Gurion University, Biomedical Engineering, Beer Sheva, Israel 2Ben Gurion University, Nuclear Engineering, Beer Sheva, Israel Brachtherapy is a tumor treatment method in which seeds containing radioactive isotopes are inserted into the tumor. The treatment is either low dose rate (LDR) or high dose rate (HDR). For LDR isotopes emitting low energy gamma radiation are used such as I-125 and Pd-103. The respective photon energies are 28 keV (main peak) for I-125 and 20 keV for Pd-103. HDR is done with Ir-192 and sometimes Cs-137. In LDR treatment, since short live isotopes are used, the seeds are implanted in the tumor and stay there till completely decayed. In HDR treatment the seeds are inserted into the tumor for a period of a few hours and then withdrawn. In the present work we have developed new seeds that can serve both as LDR and HDR. The seeds are based on the isotope Tm-170. Tm-170 emits gamma photons of energy 84 keV and x-rays of energies 52 and 59 keV. These energies are higher than those of the LDR isotopes therefore can be used for treatment of large tumors. Tm-170 half-life is 128 days, it can be used longer times and can be reactivated for reuse. Manufacturing of Tm-170 seeds is relatively simple; Tm-169 is available on the market as foils, rectangular shaped Tm-169 foils are cut to the right dimensions, inserted into titanium tubes, sealed on both ends and sent for thermal neutron activation. The neutron activation is done at a flux level and for the length of time to obtain the desired

activity. Tm-169 activation cross section is 125b. The purpose of developing these new brachytherapy seeds was not just for having this new seed with the properties as described, but as a part of the development of a new therapy method namely Auger electron therapy. The principle of Auger electron therapy is having the radiation source right at the target, the tumor cells DNA. Auger electrons have a short range, of the order of 20 nm therefore deliver their energy at the vicinity where they are emitted. They are capable of causing several DNA strand break. The auger electrons are emitted from a heavy metal atom introduced into the cell by an organic molecule to which it is linked, generally porphyrin. The metalo-porphyrin molecule enters the cell and the metal atom finds its way to the DNA. When a gamma or an x-ray photon initiates a photoelectric effect with this atom, a number of Auger electrons are emitted. The energy is deposited within a very short range and no damage is done to healthy cells. Since Tm-170 emits photons of energy 84 keV, we used Pt atoms to be the Auger electrons source. The k-edge energy of Pt is 78 keV so the probability of a photoelectric effect is large. Tm-170 emits beta rays in addition to gamma rays, at energies E-max=970 and 870 keV. We have investigated the effect of these beta rays on tumor cell killing, implanting low activity (0.3 mCi) seeds into tumors (in vivo). The range of these beta rays in water is of the order of 2 mm therefore its efficiency in treating large tumors is very small. Nevertheless we were able to cure 4 out 14 (28%) mice. 100 Direct Radiolabeling of PR81, A New Anti-MUC1 Monoclonal Antibody, With 99mTc for Radioimmunoscintigraphy of Breast Cancer M. Salouti1, H. Rajabi1, H. Babaie2, M. Rasaee3, R. Najafi2, M. Rahnama4 1Tarbiat Modares University, Medical Physics, Tehran, Iran 2The Atomic Energy Organization of Iran, Nuclear Research Center, Tehran, Iran 3Tarbiat Modares University, Biotechnology, Tehran, Iran 4Department of Microbiology, Zanjan Azad University, Zanjan, Iran Introduction: Monoclonal antibodies have been useful for immunoscintigraphic applications in clinical diagnosis since they were introduced in nuclear medicine practice. Recently PR81 was introduced as a new murine anti-MUC1 MAb against human breast carcinoma. This antibody reacts with the tandem repeat of 20-mer peptide of protein backbone, and is of IgG1 class, with an affinity of 2.19×10-8 M-1. As the first step towards the use of an antibody for imaging purposes it has to be labeled with a radioisotope. In this study we have developed a very simple, rapid and efficient method for labeling of this MAb with 99mTc. Materials and methods: The Ab reduction was performed with 2-mercaptoethanol (2-ME) at a molar ratio of 2000:1 (2-ME:MAb) and reduced Ab was labeled with 99mTc via methylene diphosphonate (MDP) as a transchelator. The labeling efficiency was determined by ITLC. The integrity of reduced MAb was checked by means of native polyacrylamide gel electrophoresis (PAGE) and gel filtration chromatography (FPLC) on superose 12 HR 10/30 (purity>99%).The amount of radiocolloids were measured by cellulose nitrate electrophoresis. In vitro stability of labeled product was checked in time intervals over 24 hrs by ITLC. Radioimmunoassay was used to test immunoreactivity of the labeled MAb. Biodistribution of the radiolabeled MAb was studied in normal BALB/c mice at 4 and 24 hrs post-injection. Results: The labeling efficiency was 94%±2.3 with high invitro stability (>%88 in 24 hrs) and less than 2.5% radiocolloids were found. There was no Ab fragmentation due to reduction procedure. Both labeled and unlabeled MAbs were able to compete for binding to the MUC1. Biodistribution studies in normal BALB/c mice showed that there was no accumulation in any organ. Conclusion: Because of no significant loss of immunoreactivity of MAb due to labeling procedure, high in vitro stability and no accumulation in vital organs, 99mTc-PR81 is a promising candidate for radioimmunoscintigraphy studies of breast cancer. References: 1. Morales AA, Crespo FZ, Gandolf GN, Escobar NI, Prez N, Hernandez JC.

Technetium-99m direct radiolabeling of monoclonal antibody ior egf/r3. Nucl Med Biol 1998; 25:25-30.

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2. Varvarigou AD, Archimandritis SC, Sekeri K, Sourlingas TG, Sivolapenko G, Paschali E. Radiochemical and radio-immunological data of 99mTc-anti-CEA labeled by two diverse methods. Nucl Med Commun 1996; 17:80-88.

3. Taylor J, Burchell J, Miles DW, Dalziel M. MUC1 and cancer. B B A 1999; 1455: 301-313.

4. Pietersz GA, Wenjun L, Krauer K, Baker T, Wrescher D, Mckenzie IF. Comparison of the biological properties of two anti-mucin-1 antibodies prepared for imaging and therapy [1997] Cancer Immunol Immunother, 44:323-328.

101 Measurement of Se-82 in order to obtain total Se content in blood of osteopenic females M.A. Chaudhri1,2, W. Kemmler3, J. Watling4 1Pakistan Council of Scientific and Industrial Research, Laboratories-Complex Lahore, Pakistan 2Institute of Medical Physics, Klinikum-Nürnberg, Nürnberg, Germany 3Institut für Medizinische Physik, Universität Erlangen-Nürnberg, Germany 4Dept. of Applied Chemistry, Curtin University of Technology, Perth, Western Australia Purpose: there is virtually no information in the literature on the involvement of Se in osteopenia or osteoporosis, especially in human beings. There are, however, some studies in animals where it is indirectly implied that the trace element Se might be involved in bone metabolism and hence in osteopenia/osteoporosis (1,2). The purpose of our investigation was to study if there is any involvement of Se with osteopenia in humans, and if it could be picked up in blood samples. Materials and methods: Subjects: 25 early postmenopausal women (1-8 years post.) mainly from central and norhtern parts of Bavaria, with osteopenia (according to WHO Classification) were randomly selected from the group participating in the research programme of the Osteoporosis Research Centre at the University of Erlangen-Nürnberg. Women were excluded if they had secondary osteoporosis, osteoporotic fractures, current or recent (last 2 years) use of medication and diseases affecting bone metabolism and inflammable disease. The Anthropometrical data and other relevant parameters of the 25 women selected were noted down. Bone measurements: bone mineral density (BMD) was measered by the well known techniques of DXA (Dual Energy X-Ray Absorptiometry) and QCT (Quantitative Computed Tomography). The DXA measurements were performed at the lumbar spine (L1-L4), the proximal femur and on the forearm by using the QDR 4500A Hologic System (Bedford, Ma., USA). QCT measurements were carried out on the lumbar spine (L1-L3) using the Somatom Plus 4 (Siemens, Erlangen). Blood sampling: on the test day participants took a standardized breakfast (6.30 am) at home and came to the laboratory by car or bus in order to avoid any physical activity. Once in the laboratory the participants rested in a sitting position for 30 min before blood samples were taken from a superficial arm vein. The samples were centrifuged for 10 minutes at a speed of 3500 revolutions per min. The plasma samples so obtained were freeze dried and sent to our analytical laboratory in Perth, Australia. Selenium determinations were carried out on the reconstituted plasma samples by using the powerful technique of Inductively-Couples-Plasma-Mass-Spectro-metry (ICPMS) which has the potential to be able to measure most elements and isotopes from Li up to U with detection limits of as low as a fraction of one ppb. However, in order to avoid interference from overlapping lines we preferred to measure the quantity of the isotope Se-82, from which we then calculated the total content of Se in the plasma samples. The quantification of Se was carried out by making use of appropriate International Certified Standard. Results: the Se contents of the plasma samples varied from 518 ppb (parts per billion or nano gram per gram) to 1187 ppb, with only three samples having Se higher than 1000 ppb. The average was 796 (SD 169). We compared these values to those given by Thorling et al (3) for Se contents of the normal Bavarian population of 1058 ppb. It was observed that 23 females, out of 25, had about 20-40% lower Se levels in their blood (plasma). Conclusions: our results clearly show, for the first time ever, that the levels of this importance trace elements Se is depleted in osteopenic females by up to 40%. We, however, are not in a

position to comment as to whether the Se shortage was a cause of osteopenia or its effect. This matter should be further investigated. But it may be worthwhile to investigate if the supplementation with Se helps reduce the frequency and severity of osteopenia/osteoporosis. References: 1. R. Moreno-Reyes et al. J. Bone Miner Res, 16 (2001), 1556-63. 2. B. Turan et al. Clin Rheumatol, 22 (2003), 432-36. 3. E.B. Thorling et al. Ann Clin Res 18 (1986) 3-7 102 Preparation of radioimmunoguided surgical pharmacy in colorectal cancer Y. Zhi, Z. Yan, L. Zhenfu, X. Bin, Z. Hong, H. Yan, G. Jin Beijing University School of Oncology, Beijing Cancer Hospital, Beijing China Objective: prepared convenience and readily and available radioimmunoguided surgical pharmacy of 125I-CL58 and evaluated its stability in vivo and vitro and its biodistribution in bearing-tumor nude mice. Methods: it was prepared by NBS (N-BromoSuccinimine) method 125I-labeled-anti-CEA (Carcinono Embryonic Antigen) antibody CL58. The stability and bioactivity of 125I-CL58 was studied. The samples were freeze-dried and the eliminated parameters were studied in whole body and in blood pool in BABL/c rats. The biodistribution of 125I-CL58 was studied in bearing human-colon cancer CL187 cells nude mice. Results: the labeling yield was more than 90% by NBS method of 125I labeled CL58 (n=10). The free 125I contents were less than 10% in placed 30 days either 125I-CL58 solution or dried power samples at 4°C. The immunoactivity of 125I-labeled-CL58 was more than 70%. The elimination of 125I-CL58 in blood pool was accorded with double chamber model, Tα=8.1h, Tβ=210h. The biodistribution results showed that: 125I-CL58 was good located in tumor. The T/NT ratios (tumor to non-tumor) had been were more than 1.0 from afterinjection of 125I-CL58 24h. At 48-72h of afterinjection 125I-CL58, the ID%/g of tumor was achieved the highest, it was well 14.70 ± 3.11. Postinjectin of 125I-CL58 7 days, the tumor to blood ratio was more than 3.0, and the tumor to the other organs ratios were all more than 5.0. The gamma image showed that the tumor was clear afterinjection 24h, and it was more clear along with the times prolong. Conclusions: it was possessed a good located capability in solorectal cancer the radioimmunoguided surgery pharmacy of 125I-CL58 prepared by NBS methods and had convenience and readily and available characteristics too. So it was thought 125I-CL58 would be a good and potential radioimmunoguided surgical pharmacy in colorectal cancer. 103 Preparation and evaluation of [142Pr/143Pr]-hydroxyapatite (Ha) and (142Pr)-DTPA for application in radionuclide therapy M.K. Das1, K.V.V. Nair2, A. Mukherjee2, H.D. Sarma3, S. Pal4 1Board of Radiation & Isotope Technology, Radiopharmaceuticals, Kolkata, India 2Bhabha Atomic Research Centre, Radiopharmaceuticals, Mumbai, India 3Bhabha Atomic Research Centre, Radiation Biology & Health Physics, Mumbai, India 4Variable Energy Cyclotron Centre, Regional Radiation Medicine Centre, Kolkata, India 142Pr (t½ 19.12h, Eβmax 2.16 MeV) and 143Pr (t½ 13.57d, Eβmax 0.937 MeV) are radioisotopes of good potential for radionuclide therapy (RNT). We have found that 142Pr and 143Pr can be produced by neutron irradiation at the rate of 2.5GBq/mg of Pr at the end of irradiation (EOI) and 0.9 MBq/mg of target at 7 days post EOI, respectively and the latter product can be obtained in no-carrier-added (nca) form. These data encouraged us to prepare and evaluate two radiopharmaceuticals. Hydroxyapatite (HA) particle suspension was labeled with 142Pr and 143Pr by addition of [142Pr/143Pr]-PrCl3 at pH 5 with radiochemical yield of 99%. In vitro studies showed the product to be stable at ambient temperature, retaining more than 96% radiochemical purity (RCP). Intra-articular injection in rats revealed more than 99% retention of

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[142Pr]-HA in the knee joint 48 hours post injection. Biodistribution of [142Pr]-HA in rats was also studied with encouraging results, confirming the suitability for radiosynovectomy. There is a greater prospect of utility of 142Pr for therapies requiring rapid rate of deposition of absorbed dose as in endo-vascular radionuclide therapy (EVRNT). [142Pr]-DTPA would behave like any other established metal DTPA complexes with fast clearance via the urinary system. It was prepared by addition of [142Pr]-PrCl3 to DTPA solution in dilute alkali and with ligand metal ratio of 2:1. At pH 7.5-8 the radiolabelling efficiency was greater than 94%. The complex was characterized by thin layer chromatography (TLC) (RC purity >98%) and found to be stable during the study-period of 2 days. Further evaluation of 142,143Pr-labelled compounds is strongly advocated for RNT. Track 5 – Session 1b: Medical Isotope Applications II 104 Preclinical application of Re-188-tin colloid for treatment of mouse tumor model with peritoneal effusion J.M. Jeong1, Y.N. Kim1, Y.J. Lee1, H.Y. Lee1, Y.J. Kim1, M. Son2, D.S. Lee1, J.Chung1, M.C. Lee1 1Seoul National University College of Medicine, Nuclear Medicine, Seoul, Korea 2Dong-A Pharmaceutical Co. Ltd., Research Laboratories, Yongin, Korea Objectives: Radiocolloids have been used to control malignant ascites. 188Re-tin colloid has been reported as an ideal agent for radionuclide therapy. This experiment was designed to validate the usefulness of 188Re-tin colloid for treatment of malignant peritoneal effusion in animal model. Methods: 188Re-tin colloid was prepared by reaction of generator-eluted 188Re-perrhenate (30 mCi/0.8 ml) with tin colloid kit (10 mg SnCl2·2H2O, 1 µg ascorbic acid, 0.2 ml 0.1 M HCl) for 2 hr at 100°C. Labeling efficiencies were checked by ITLC-SG/saline. To obtain peritoneal effusion models, 7 × 106 Sarcoma-180 cells were injected intraperitoneally into each ICR mouse and grown for 12 days. 188Re-tin colloid was intraperitoneally injected into each tumor-bearing mouse. The doses were 0.5, 1, and 2 mCi per 30 g body weight. Distributions of 188Re radioactivities in the mice' bodies were checked using gamma camera at 24 hr post injection. Each group was consisted with 9 mice. The effects of 188Re-tin colloid to survival time and body weight were monitored. Statistical analysis was performed using SPSS version 10.7. Results: Labeling efficiency of the 188Re-tin colloid was higher than 99%. Homogeneous distribution of radioactivity in the abdomen was found in 24 hr images of treated mice. Significant decrease of body weight due to radiation toxicity in 2 mCi group was observed 6 days after treatment (p=0.009 by Mann-Whitney test). Survival times were analyzed using Kaplan-Meier test. Survival times of 1 mCi group (10.3 ± 5.1 days, p=0.059) and 2 mCi group (6.7 ± 1.5 days, p=0.651) were not significantly different from control group (6.8 ± 2.5 days), while 0.5 mCi group showed significantly increases survival time (16.8 ± 9.6 days, p=0.004). Conclusions: 188Re-tin colloid showed homogeneous distribution in the abdomen of peritoneal effusion mice model and excellent life-extending effect at the dose 0.5 mCi/30 g-mouse (equivalent to 80 mCi/60 kg-human by BSA). 105 Preparation and evaluation of 125I-Cl58 for radioimmuno-guided surgery of colorectal cancer Z. Yang, Z. Li, B. Xu, H. Zhang, J. Gu Peking University School of Oncology & Beijing Cancer Hospital, Beijing, China Objective: Radiolabeled monoclonal antibodies have been playing an important role in radioimmunoguided surgical. CL58, anti-CEA (CarcinoEmbryonic Antigen) antibody, was labeled with 125I in convenient and available method, and in vitro and in vivo characterizations were carried out.

Methods: 125I-CL58 was prepared by NBS (N-BromoSuccinimine) method, then was freeze-dried for storage, which is convenient for clinical use. The stability and bioactivity of 125I-CL58 was tested. In addition, the biodistribution in human-colon cancer CL187 cells bearing nude mice and the eliminated parameters from blood pool in BALB/c mice were determined. Results: The labeling yield of 125I-CL58 was more than 90% by NBS method (n=10). Both of 125I-CL58 in solution and in freeze-dried powder were stable, which radiochemistry purity was still more than 90% after storage at 4°C for 30 days. The immunoactivity of 125I-CL58 was more than 70%. Pattern of blood clearance of 125I-CL58 was defined as two-compartment model, with T½α and T½β calculated to be 8.1 h and 210 h, respectively. The biodistribution results showed that 125I-CL58 was well accumulated in tumor, as T/NT ratios were more than 1.0 from 24 h postinjection of 125I-CL58. The ID%/g of tumors was achieved the highest at 72 h postinjection with 14.70±3.11. The radioactive ratios of tumor to blood were more than 3.0 on the 7th day postinjection of 125I-CL58, and the ratios of tumor to other organs were all more than 5.0. The clear images of xenografted tumors were obtained at 24 h, and it further improved along with the time. Conclusions: The 125I-CL58 prepared by NBS method was stable in vitro. The biodistribution and γ imaging results showed that 125I-CL58 was an ideal candidate for radioimmunoguided surgical of colorectal cancer. 106 Development of a new isotopic Methodology for thyroid metabolism investigations A. Hantson, M. De Meyer, N. Guérit Faculté Polytechnique de Mons, Applied Chemistry and Biochemistry, Mons, Belgium Synthetic molecules labeled with stable isotopes, implemented as biological tracers, bring new means of metabolic investigations, pharmacodynamic studies and clinical diagnostic tests. The major interest of stable isotopes labeled chemicals is obviously their harmlessness to the human organism, contrary to the radioactive products. For understandable ethical reasons, the use of the latter is banned for in vivo tests on children; consequently, alternative methods of metabolic investigations or diagnosis must be researched. The principal objective of this experimental study is the development of a new tool for the study of the thyroid metabolism based on double isotopic dilution technique with the use of two isotopomers of the same hormone enriched with distinct carbon 13 contents. The successive stages of the methodology are described below: 1.Optimized synthesis of the thyroid hormones being used as biological tracers or analytical internal standards (thyroxine: T4-13C9 and 13C6; 3,3',5-triiodothyronine: T3-13C9) with starting material (L-tyrosine) enriched with carbon 13; 2.Incorporation of the tracer (13C6-T4) by the patient and collect of samples of plasma over a given period of time; 3.Internal standard addition to plasma (T4-13C9 or T3-13C9); 4.Solvent extraction, SPE and LC purification of the thyroid hormones (endogenous, tracer and standard) of the plasma; 5.Derivatization (with methanolic HCl and HFBA( of the thyroid hormones for GC-volatilization at 280°C; 6.Analysis and quantification by gas chromatography coupled with mass spectrometry (by follow-up of the specific ions of each isotopomer), monitoring of (m/z) values 970/979 and 976/979 for thyroxine. The instrumental optimization of GC-MS analytical protocol - namely chromatographic separation and management of the ions of mass in SIR mode - was worked out for the analysis of traces of T3 and T4. The limit of detection is 100 pg (s/n = 3.0). A first implementation in in vivo tests of T4-13C9 as a metabolic tracer was carried out under veterinary control on cats and rabbits thanks to the collaboration of the Clinical Department of Biochemistry of Royal Infirmary of Edinburgh. They enabled us to prove the feasibility of the methodology (incorporation of the probe and its temporal follow-up) and the possibility of using these tracers as probes for human beings.

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107 Specific identification to lymphoma cell and biodistribution in nude mice bearing human lymphoma with radioiodine labeling tyramine immunoglobulin frame region antisense oligo-nucleotide R.F. Wang, J. Shen, C.L. Zhang, F.Q. Guo Peking University First Hospital, Nuclear Department, Beijing, China Objectives: To select immunoglobulin (Ig) heavy chain variable region gene (VH) framework region 1 (FR1) of VH1 family verified to be a major determinant of malignant phenotype of VH 1 family B-cell lymphoma as a suitable target to all of VH1 family B-cell lymphoma and validate the potential of using radiolabeled Ig VH FR1 antisense oligonucleotides (ASON) as an imaging agent or antisense therapeutic radiopharmaceuticals in lymphoma. Methods: Probe labeling and biodistribution were studied in the present report. A 18-mer partial phosphorothioate oligonucleotide sequence was synthesized and grafted in 5’ with a tyramine group which was further radioiodinated. The Namalwa (VH 1 family) and HL-60 cell lines were transducted with liposome-mediated 125I-FR1-ASON, and the transduction efficiencies were calculated. Liposome-mediated 131I-FR1-ASON and 131I labeled sense oligonucleotides were injected intratumorally into tumor-bearing BALB/c mice (6 weeks after inoculation of 107 Namalwa cells). Biodistribution was monitored by sequential scintigraphy and organ radioactivity measurement at 24 h after injection. Results: The 5’tyramine group allowed specific and stable radiolabelling of the ASON with radioiodine. The transduction efficiency in Namalwa cell lines reached (26.8±1.54)% that was higher than HL-60 cell lines. When antisense probe injected intratumorally into mice grafted with Namalwa cell line, images show the tracer accumulate in tumor. Conclusion: The findings of our study suggest that IgVH FR 1 gene is a suitable target for radiolebeled ASON and leads to the expectation of a new type of radiopharmaceuticals with unique specificity. 108 Monte-Carlo dosimetry simulations of mono- and bi-isotopic radioactive sources used in prostate brachytherapy V. Nuttens, S. Lucas University of Namur Physic (LARN Lab)(FUNDP), Namur, Belgium Cancer is one of the greatest diseases of this last 20 years. Nuclear physics has been of a great importance in its treatment by the use of external beam radiotherapy, brachytherapy, targeted radiotherapy, ... The Ultra Low Dose Rate (ULDR) brachytherapy have been developed for localized cancer such as prostate cancer where healthy tissues have to be preserved carefully (rectum, urethra, bladder). It consists in the implantation of radioactive seeds in the vicinity of the tumor. Developments in ULDR brachytherapy have led to use two kinds of radio-isotopes: Iodine-125 and Palladium-103. Iodine is usually preferred by physicians because of its good deposited dose homogeneity avoiding hot and cold spots in the target volume that are more often observed with palladium seeds. However, palladium delivers doses at a higher rate than iodine allowing the treatment of more aggressive tumor. In order to benefit from this advantage while avoiding cold spots, a new configuration of source composed of both radio-isotopes is considered. Theoretical dosimetry studies by Monte-Carlo simulations have been performed on this new bi-isotopic source. It shows advantages in comparison to mono-isotopic sources. Adjusting the relative activity of Iodine-125 and Palladium-103, one can get a high dose rate at short AND long distances. The difference in the half-lives is also a great advantage because it allows to have a dynamic dose rate versus distance and time. Combination of other potential radio-isotopes will be presented.

109 Argentine production of 125I seeds for tumor brachytherapy G. Baro, J. Kiefer, H. Gutierrez, R. Ughetti, J. Nicolini Laboratories Bacon S.A.I.C., Radiochemistry Production, Buenos Aires, Argentina This work presents the Argentine production of 125I seeds with a quality similar to those internationally used. These seeds, which are widely used for tumor brachytherapy, have been produced during the last 2 years with a commercial denomination of Braquibac TM, are covered by Argentine Patent n° 02010 1884. The seeds are similar to Amersham model 6711, widely used throughout the world. The seeds manufacture is carried out with GMP, under ISO 2919 regulation, which qualifies the seeds as a sealed source and ISO 9978 which determines the limits for the external removable activity, which is much lower than the upper limit of 185 Bq. The isodose calculations, carried out by the Regional Dosimetry Group of the Argentine Atomic Energy Commission, showed that our seeds and those of Amersham model 6711, exhibit isodose curves which can be almost exactly superimposed. During the production period of 2 years, 27500 seeds have been manufactured, controlled and sold. The seeds production is certified by the International Standardization Organization, the Argentine Health Authorities and the Nuclear Regulatory Authority. This production has shown to be important, since it allows supplying a product with international quality at a lower price. 110 Elemental composition of human liver samples with XRF M.A. Chaudhri 1, 2 , M.N. Chaudhri 1, M. Koulmanda 3

1Pakistan Council of Scientific and Industrial research, Laboratories-Complex, Lahore 2Department of Medical radiation Physics, Institute of Medical Physics, University of Erlangen-Nuernberg, Erlangen, Germany 3The Walter & Eliza Hall Institute of Medical Research, Melbourne, Australia The elemental composition of liver samples obtained at autopsies from people dying of different diseases have been measured using the technique of X-Ray Fluorescence Analysis (XRF). Normally more than one sample was obtained from different parts of the liver of each patient, especially if the liver was found to be diseased. The blood was removed from the samples, they were chopped into small pieces with an ultra clean non-metallic knife and freeze dried. The samples were then crushed in an ultra-clean grinder and pelleted in a suitable form for use in a commercial XRF system. For estimating the absolute concentrations of different elements, the NIST-Bovine-Liver Standard, was used and pelleted in the same fashion. A number of elements. Na, Mg, Al, Si, P, Cl, S, K, Ca, Ti, Cr, Mn, Fe, Cu, Zn, Rb, Sr, Ba, Pb, were detected in all the samples and their concentrations determined. No matrix correction was necessary, as the matrices of the samples and the Standard were assumed to be very similar. The results obtained are compared to the concentrations of these elements in the livers of normal subjects, and might throw some light on the causes of the diseases with respect to trace element imbalances. 111 Free-GES head gamma-knife for stereotactic surgery T.X. Fei, Y. Ding, W.J. Dong Shenzhen Linden Science & Technology Development Co., Ltd. The report describes the FreeGS gamma knife – spatial orientation equipment, which is a leading product of the Shenzhen Zunrui Science & Technology Development Co., Ltd., as well as experience of its clinical use. FreeGS head gamma knife realizes so called stereotactic radiosurgery, which uses multiple beams of gamma radiation converging in three dimensions from thirty encapsulated Co-60 sources to focus precisely on a small volume, permitting intense doses of radiation to be delivered to that volume safely. With the three-dimensional coordinated headframe, gamma knife locates intracranial focus precisely and provides gyroidal irradiation of the

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target. High dose rate irradiation destroys the target, while surrounding normal tissues and important organs are spared with little injury, so as to carry the point of radiosurgery. Treatment indications for the stereotactic radiosurgery are as follows: 1. Intracranial blood vessel malformation: intracranial arteriovenous malformation, intracranial aneurysm, cavernous angioma etc. 2. Intracranial benign tumors: meningioma, pituitary adenoma, acoustic neurinoma, Pinealoma, craniopharyngioma, chordoma, trigeminal neurinoma, hemangioblastoma, neurilemoma, etc. 3. Functional disorder: parkinsonism, trigeminal neurialgia, inflexible pain, epilepsy, mental diseases, etc. 4. Post open-cranial surgery remnants. 5. Recrudescent tumor after regular treatment. 6. Intracranial tumors or vessel malformation with little probability for open-cranial operation. Using of Gamma knife treatment technique allows avoiding of the risk of open-cranial surgery and consequence functional disorders. It is highly accurate and safe, easily accepted by elder or feeble patients, gives satisfying curative effects, with no sequela, or rare complication and high life quality. It provides short period of treatment, permitting early normal life after short period of hospitalization and rehabilitation therapy that is accordingly less expensive. Besides, it allows using of multiple focuses with one-time radiation, or repeating therapies. Track 5 – Session 2 Therapy – BNCT and Radioisotope Therapy 112 Neutron capture therapy using liposomal 10B targeting of tumour cells and tumour vasculature G.C. Krijger1, M.M. Fretz2, V.A. Nievaart1,3, U.D. Woroniecka1, W. Jiskoot2, G. Storm2, R.L. Moss3, G.A. Koning1 1Delft University of Technology, Radiation, Radionuclides and Reactors, Delft, The Netherlands 2Utrecht University, Pharmaceutics, Utrecht, The Netherlands 3European Commission, Joint Research Centre, Petten, The Netherlands Boron neutron capture therapy for cancer treatment requires the specific accumulation of high 10B quantities in tumours. The therapy is based on the induction of radioactivity by local irradiation with thermal neutrons. We have adopted two different tumour targeting approaches. In the first one, ovarian carcinoma cells (OVCAR-3) are targeted directly. In the second approach, the angiogenic endothelium is targeted to cause damage to tumour blood vessels and, subsequently, tumour regression. For this angiogenic endothelium, human umbilical vein endothelial cells (HUVEC) were used as model cells. For targeting 10B-containing liposomes to OVCAR-3 or HUVEC, a monoclonal antibody or an RGD peptide, respectively, was coupled to the liposomes. In both approaches, liposomal targeting devices were used that efficiently retained the hydrophilic boron compound dodecahydrodo-decaborate, i.e. [10B12H12]2-. Their internalization by tumour cells and endothelial cells was shown by confocal microscopy. 10B accumulation ratios in both cell types were in favor of the targeted liposomes compared to non-targeted liposomes. In vitro irradiations with thermal neutrons showed strong inhibition of cell growth of 10B targeted OVCAR-3 and HUVEC. These results show that targeted liposomes hold promise for the field of neutron capture therapy. 113 In-phantom dosimetry for boron neutron capture therapy (BNCT) G. Gambarini1, V. Colli1, S. Gay1, C. Petrovich2, G. Rosi3, M. Valente1 1Physics Department of University, Milano, Italy 2FIS-NUC, ENEA, Bologna, Italy 3FIS-ION, ENEA, Casaccia (Roma), Italy In-phanom measurements of physical dose distributions are very important for BNCT planning validation. During exposure to thermal or epithermal neutrons, the absorbed dose in tissue is

released by the various components of secondary radiation. Therefore, it is necessary to determine the spatial distributions of the absorbed dose, separating the various contributions, because they have dissimilar biologic effect. The spatial trends of the different dose components and their relative contributions in each position depend on the beam geometry and also on the size and shape of the irradiated volume. Gel dosimeters have demonstrated to be able to image the dose distribution of each radiation component. The measured doses are. (a) the gamma dose, due to gamma rays induced by thermal neutron reactions with hydrogen in the tissue itself and with various isotopes in the structures around the beam.; (b) the neutron dose, mainly due to recoil protons owing to scattering reactions of epithermal and fast neutrons; (c) dose from protons emitted in reactions of thermal neutrons with nitrogen; (d) dose due to α particles and 7Li ions emitted in 10B(n,α)7Li reactions; (e) electron dose in the case of presence of 157Gd; in fact, the gamma rays emitted in the reaction 157Gd(n,γ) are measured together with those of point (a), and the dose due to internal conversion and Auger electrons is imaged separately. A method has been settled for achieving the dose images in phantoms also having suitable non-homogeneity, well fitting neutron transport conditions. The proposed technique for in-phantoms dose imaging and profiling utilizes gel dosimeters in form of layers, imaged with an optical method by means of a CCD camera. A method for dose mapping, and for separating the contributions of the secondary radiation, with thermoluminescent dosimeters (TLD) has been developed too. Fluence measurements with activation techniques and Monte Carlo simulations are performed in order to confirm the reliability of the methods. 114 Pharmacokinetics and proteomics for BNCT clinical trials P. Mauri1, F. Basilico1, A. Wittig3, C. Ferrari2, A. Zonta2, W. Sauerwein3 1CNR-ITB, Milan, Italy 2IRCCS, Pavia, Italy 3University of Essen, Radiotherapy, Essen, Germany In the development of synthesis and delivery drug strategy, it is of primary importance to determine the absorption levels and localization of an administered drug in biological fluids and tissues, in order to be able to characterize its potential utility, check its concentration in the tumor and optimize its administration. For this reason, efforts have to be made to measure pharmaco-kinetics and to be able to quantify drugs in blood samples and in tissue extracts. In addition, to understand the biochemical and physiological differences between tumor cells and their normal counterparts and to be able to use these differences in compound design, synthesis and targeting, it is very important to investigate protein profiles related to different physiological states (normal and tumoral) as well as to study protein-protein interactions and protein modifications. For these reasons, we have developed an integrated approach for characterization and quantification of boron compounds in biological samples and the related protein profiles. Although several 10B containing compounds belonging to different chemical families have been synthesized, there are still only two products currently used in BNCT trials for the treatment of glioblastoma multiforme and melanoma: BSH (closo-undecahydro-1-mercaptododecaborate) disodium salt and BPA (boro-phenylalanine). In particular, BSH and BPA derivatives were analyzed by means of ion trap mass spectrometry, using direct injection of samples. This approach allows their complete characterization in a short time (about 2 min for analysis) and high sensitivity (limit of detection: 50 fmol). Moreover, for the same samples, protein analysis is performed using the LC/LC-MS/MS (also called MudPIT, Multidimensional Protein Identification Technology) approach. It consists of one single direct analysis of peptides obtained from digestion of a protein extract. Peptides are separated first by ion exchange and then by reversed-phase chromatography. The eluted peaks from 2DC (LC/LC) are analyzed directly by mass spectrometry to obtain molecular weight and fragmentation of each peptide. This proteomic approach allows simultaneously the separation of digested peptides, their sequencing and then the identification of related proteins present in the samples (cell lines and urine). Using this methodology it is also possible to

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detect protein modifications due to administration of boron compounds. The main objectives of a "metaboleomics and proteomics" integrated approach, is to develop and apply innovative methodologies for increasing sensitivity, accuracy and resolution to accelerate the development of tumor targeting drugs and drug delivery systems suitable for Boron Neutron Capture Therapy. 115 Boron imaging: A European Research Project A. Wittig1, J. Michel2, K. Zierold3, H. Arlinghaus4, R. Moss5, R. Huiskamp6, G. Kaizer7, C. Loquai8, P. Therasse9, W. Sauerwein1 1University of Essen, Radiotherapy, Essen, Germany 2University of Reims, INSERM, Reims, France 3Max Plank, Molecular Physiology, Dortmund, Germany 4Univeristy of Munster, Munster, Germany 5IE/JRC, HFR, Petten, Netherlands 6Nuclear Research and Consultancy Group (NRG), Petten, Netherlands 7Dept. of Surgery, University Hospital Essen, Essen, Germany 8Dept. of Dermatology, University Hospital Essen, Essen,Germany 9EORTC Data Center, Brussels, Belguim Improvement of anti-cancer therapies, therapeutic and diagnostic strategies rely on the ability to selectively deliver compounds to target cells. Imaging of such targeting compounds and knowledge of their distribution as well as that of intrinsic elements and molecules in cells is of great interest. The aim of this European project is to develop tools for imaging and quantifying of atoms and molecules within tissues and single cells. Electron energy loss spectroscopy (EELS), time of flight secondary ion mass spectrometry (TOF-SIMS) and laser secondary neutral mass spectrometry (Laser-SNMS) - each capable of simultaneously detecting all masses with very high sensitivity and sub-cellular resolution - were developed to be used for imaging and quantifying atomic species in biological samples. Prompt gamma ray spectroscopy was used to assess the boron concentration in macroscopical volumes. All tissues were characterised histopathologically. For analysis of cell cultures and tissues dedicated cryo-fixation methods are mandatory. With TOF-SIMS and Laser-SNMS high-resolution elemental images and mass spectra were obtained in cells and tissues. The measurement of the Na/K ratio, which had to be similar to the one of living cells, was used to select cells for detailed investigation. Incubation of melanoma cells with the boronated compound BSH resulted in a boron signal inside the cells, which was lower than the one outside cells in the culture medium. The results with EELS give evidence of an inhomogeneous spot-like distribution of boron inside single cells. Successful sample preparation preserving the chemical integrity of cells has been demonstrated. Imaging of boron inside single cells was possible with the 3 dedicated methods used, thus demonstrating their suitability for imaging elements in biological material. Collection and storage of samples from patients in clinical trials are special aspects of translational research. The application of a boronated drug prior to surgery has no individual benefit for the patient. Successful handling of the related ethical, legal and regulatory aspects need the support of a dedicated organisation such as the EORTC. The realisation of such research requires an especially close interdisciplinary collaboration between clinicians and basic scientists. 116 BNCT facilities around the world: is there an optimal approach? R. Moss1, S. Nievaart1, A. Wittig2, F. Stecher-Rasmussen2, W. Sauerwein2 1IE/JRC, HFR, Petten, The Netherlands 2University of Essen, Radiation Oncology, Essen, Germany In Europe, there are currently 5 different centres in 5 different European countries actively performing clinical trials on BNCT. The trials are performed at the following nuclear research reactors: the HFR Petten (Netherlands), the FiR-1 reactor Otaniemi (Finland), the R2-0 reactor Studsvik (Sweden), the LVR-15 reactor Rez (Czech Republic) and the TRIGA Mark II reactor Pavia (Italy). To-date, the centres have together treated more than 100 cancer

patients. Apart from 2 liver cancer patients treated at Pavia, all other cases have been brain tumour patients, primarily glioblastoma multiforme. Elsewhere in the world, patient treatment has continued in Japan (at the JAERI and KURRI facilities) and at the only facility outside the northern hemisphere, patients have been treated at the Bariloche reactor in Argentina. In the USA, however, clinical trails are currently halted, but plans to continue are under discussion. Despite the number of available BNCT facilities, each one is located at a different type of nuclear research reactor and consequently, no two beams are identical. The question is thus posed as to whether one beam is more advantageous than another or whether any of the beams approaches that of the so-called optimal beam, if it exists. It will be seen that the optimal beam is not only reactor dependent but also application dependent, i.e. the type of tumour to be treated, e.g. superficial or at depth. 117 Clinical trials of the EORTC BNCT Group W. Sauerwein1, A. Wittig1, K. Hideghety2, P. Paquis3, K. Haselsberger4, C. Goetz5, J. Heimans6, A. van Loenen7, S. Grabbe8, C. Broelsch9, P.(. Therasse, F. Stecher-Rasmussen11, R. Moss12 1Dept. of Radiation Oncology, Universitätsklinikum Essen, Essen, Germany 2Dept. of Radiotherapy, University Kaposvár, Hungary 3Dept. of Neurosurgery, Hôpital Pasteur CHU, Nice, France 4Dept. of Neurosurgery, Karl-Franzens-University, Graz, Austria 5Dept. of Neurosurgery, Klinikum Großhadern, Munich, Germany 6Dept. of Neuro-oncology, Vrije University medical cemter, Amsterdam, Netherlands 7NDDO Oncology, Amsterdam, Netherlands 8Dept. of Dermatology University Hospital Essen, Essen, Germany 9Dept. of Surgery, University Hospital Essen, Essen, Germany 10EORTC Data Center, Bruxelles, Belgium 11NCT Physics, Alkmaar, Netherlands 12Joint Research Centre, Institute for Energy, Petten, Netherlands Clinical research on boron neutron capture therapy (BNCT) requires the development of special concepts as the binary character of this treatment modality and the experimental character of this therapy has to be considered. The aim of this project is to develop and conduct strategies for the evaluation of BNCT as an oncological treatment modality. The EORTC BNCT Group has applied the tools of modern clinical research on BNCT to establish a system of controlled prospective clinical trials, which covers early translational research, phase I and phase II evaluations up to efficacy testing. The trials are designed in a way that the concepts can be applied to similar questions in the future. Protocol EORTC 11001 (translational research and early phase I) aims to identify tumor entities that may benefit from BNCT by evaluating tissue uptake of BSH or BPA but also the potential and toxicity of a combined application of BSH and BPA. Data of BSH and BPA-uptake in tissues and in individual cells are collected. The study protocol 11961 evaluates as a phase I trial the healthy tissue tolerance of brain of patients suffering from glioblastoma multiforme after an irradiation with BNCT using the compound BSH. The systemic toxicity of BSH and the early and late radiation toxicity of the combined modality are evaluated separately. Protocol EORTC 11011 (phase II) evaluates the anti-tumor activity as objective response to BNCT using the compound BPA in metastatic melanoma. As a secondary endpoint, toxicity and pharmacokinetics of BPA after repeated administration and the toxicity of BNCT are evaluated. As translational aspect it also includes a biodistribution study. This trial is conducted in close collaboration with the BNCT-group at Harvard Medical School and Massachusetts Institute of Technology (MIT) being the first 2-centre trial on BNCT. In protocol 11961, treatment of 4 cohorts of patient is completed and data have been evaluated. No reproducible and dose limiting toxicity was observed. First results from protocol 11001 and 11011 are now available. For protocol 11011 despite slightly different beam characteristics of the irradiation facilities at Petten and MIT the concepts of prescribing and reporting of dose as well as further physical and medical details could be adjusted as to a common analysis of the trial results will be possible. The irradiation dose level, which has been reached within the dose escalation study 11961 is still below the maximal tolerable dose.

5ICI April 25 – 29, 2005 35

The conceptual strategy has proven feasibility and potential. The recent results of the ongoing trials 11001 and 11011 will be presented. Special attention will e given to safety and quality assurance aspects considering an experimental treatment at a non hospital based facility, i.e. a nuclear research reactor. A strategy has been established to enter BNCT in clinics by creating a system of prospective clinical trials. 118 Boron concentration imaging for BNCT S. Altieria,b , A.Braghierib, S. Bortolussia, P. Bruschia, F.Fossatia, P. Pedronib, T.Pinellia,b, A. Zontac, C.Ferraric, U.Pratid, L.Rovedae, S.Barnif, P.Chiarif, R.Nanof

aDipartimento di Fisica Nucleare e Teorica dell’Università, via Bassi, 6 27100 Pavia, Italy

bIstituto Nazionale di Fisica Nucleare-Sezione di Pavia, via Bassi, 6 27100 Pavia, Italy

cDipartimento di Chirurgia dell’Università, via Aselli, 45 Pavia, Italy dChirurgia Sperimentale e Tecnologie Chirurgiche Innovative IRCCS Policlinico S. Matteo, Pavia, Italy eChirurgia Epato-Pancreatica IRCCS Policlinico S. Matteo, Pavia, Italy f Dipartimento di Biologia Animale e Centro di Studi per l’Istochimica IGM-CNR, Pavia, Italy A precise knowledge of the boron concentration, both in tumor and healthy tissues, is an essential requirement for the BNCT treatment of cancer. Many methods can be used to detect the boron signal coming from biological samples, but it is very important to know what type of tissues are present in the sample. In the case of liver metastases, for example, tumor cells are disseminated through the healthy tissues. Tumor cells, normal hepatocytes, blood cells and necrotic material can be simultaneously present inside a metastatic nodule having a diameter of a few millimeters. In this paper we show the results of the analysis of tumor samples from human liver infused by BPA that was performed using neutron radiography. We have found that the boron concentration is very different in the various biological materials. This demand to take into account the morphology of the sample for the correct evaluation of the boron concentration.

Track 5 – Session 3: Targeted Alpha Therapy (TAT) 119 Metallic α-emitting radionuclides for TAT G. Beyer CERN, Switzerland The table of isotopes does not provide a large number of α-emitting radionuclides that are in principle suitable for targeted alpha therapy in humans. Most relevant are: 225Ac (10 d), 224Ra (3.66 d), 223Ra (11.4 d), 213Bi (45.6 m), 212Bi (60 m), 211At (7.2 h), 149Tb (4.1 h) and 255Fm (20.1 h). With the exception of 211At (7.2 h) these are generally metallic radionuclides. The success of the chelated bio-conjugates (peptides and monoclonal) radio-labelled with 90Y or 177Lu has initiated simultaneously the interest in metallic alpha emitters, especially in the trivalent state, because they can be seen as analogues of these rare earth isotopes. In this presentation the author will analyse the different production routes based on the results of the previous workshops and based his own experimental work. The scheme in Fg.1 illustrates the main production modes for the most important isotope of this class, 225Ac. Production routes are

via 229Th, that could be separated from the available 233U stock pile, or via triple neutron capture breeding from 226Ra, or from photon, neutron or proton induced reactions on the natural 232Th or 230Th. Other production routes leads to the mother nuclide of 225Ac, the 225Ra via the 226Ra (γ,n) 225Ra process. The often mentioned direct production mode makes use of the 226Ra (p,2n) 225Ac process using an ordinary cyclotron. Very promising seems to be the spallation process, using either depleted 238U or natural 232Th targets, that allows the simultaneous harvesting of both 225Ra and the 225Ac. Off-line and on-line production modes are possible, including isotope separation techniques [1,2]. B.Allen [3] proposed the lanthanide isotope 149Tb for TAT, having the advantage of a longer half-life compared to 213Bi, the lower alpha energy (3.97 MeV) and the close chemical properties related to 90Y or 177Lu. At the ISOLDE facility at CERN, we prepared batches of up to 500 MBq 149Tb by combining spallation and on-line mass separation process followed by a cation exchange chromatography using γ-HIBA as eluent. The obtained 149Tb preparations showed excellent behavior in labeling of monoclonal antibody conjugates. The most promising heavy actinide 255Fm is usually not considered for research activities in TAT. The initiative of the NIIAR, Dimitrovgrad (O.I.Andrejev et al [4]) to make this isotope available for research activities will be mentioned. The two radium isotopes 223Ra and 224Ra have great potential in TAT as well. Suitable groups that can bind the bivalent Ra stable to bio-conjugate constructs are under development. They are available from the 227Ac and 228Th decay chains, using known generator systems. These very different production routes for the metallic alpha emitters will be critically compared emphasising the related problems of legislation, financing, safety and security as well as quality aspects. [1] G.J.Beyer et al., Comparison of the Biodistribution of 225Ac and Radiolanthanides … , Isotopenpraxis 26, 111, (1990) [2] G.J.Beyer et al. Biokinetics of monoclonal antibodies labelled with radio-

α

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213Po 4.2 µs

209Pb3.253 h

209Bi

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221Fr 4.90m

217At 32.3 ms

213Bi 45.9 m

209Tl 2.16 m

233U 159200 y

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229229Th Th 7880 y7880 y

225Ra 14.8 d

97.8 %

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27 d238U,232Th (p, spall.)

226Ra (p,2n) 226Ra (γ, n)

230Th (γ,n)226Ra (3n,2ß)

232Th (p,4n) 229Pa

Fig.1233U-decay chain and most relevant production routes for the radionuclides

α

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ß-ß-

213Po 4.2 µs

209Pb3.253 h

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229229Th Th 7880 y7880 y

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97.8 %

232Th (n,γ) 233Pa ß-

27 d238U,232Th (p, spall.)238U,232Th (p, spall.)

226Ra (p,2n)226Ra (p,2n) 226Ra (γ, n)226Ra (γ, n)

230Th (γ,n)226Ra (3n,2ß) 230Th (γ,n)226Ra (3n,2ß)

232Th (p,4n) 229Pa

Fig.1233U-decay chain and most relevant production routes for the radionuclides

36 April 25 – 29, 2005 5ICI

lanthanides and 225-Ac …. J.Lab.Comp.Radiopharm. XXXVII, 529 (1995), [3] B.Allen and N.Blagojevic, Alpha- and beta emitting radionuclides in targeted cancertherapy, Nucl.Med.Commun. 17, 40, 1996 [4] O.I.Andrejev et al.,Production of highly pure Ei and Fm preparatins, this conference, ICI-0182 120 Targeted α radiation and γ rays induce distinct and mutation status specific responses in human leukemic lymphocytes as revealed by gene expression profiling S. Martin1, R. Kronenwett2, K. Vandenbulcke3, C. Apostolidis1, A. Morgenstern1, S. Kliszewski2, F. Offner4, R. Haas2 1European Commission, JRC, ITU, Nuclear Chemistry/Alpha-immunotherapy, Karlsruhe, Germany 2University of Duesseldorf, Hematology, Oncology, Clinical Immunology, Duesseldorf, Germany 3University of Gent, Radiopharmacy, Gent, Belgium 4University of Gent, Hematology, Gent, Belgium Alpha-immunotherapy (AIT) specifically targets tumor cells using alpha particle emitting isotopes conjugated with monoclonal antibodies. The alpha emitter 213Bi has a high linear energy transfer and a short path length in tissues compared with gamma-rays, which allows him to kill cells by few nuclear hits, sparing healthy surrounding cells. As 213Bi-based targeted AIT evolves as a new treatment modality currently proved in clinical trials for acute leukemia, non-Hodgkin's lymphoma, malignant melanoma and preclinically for chronic lymphocytic leukemia (CLL) and stomach cancer, our aim was to understand the molecular effects of 213Bi-immunoconjugates. We assessed gene expression profiles of blood lymphocytes from 12 patients (pts) with CLL using cDNA arrays comprising 1,185 genes. Cells treated in vitro with 213Bi-CD20 or an equivalent dose of gamma radiation (60Co) were intraindividually compared with non-treated cells. According to the two variants of CLL, with mutated (6 pts) or unmutated (6 pts) rearranged immunoglobulin genes (VH), we also aimed to verify whether radiation effects are mutation status specific. At the time of gene expression profiling, a median of 4% and 6% of cells had undergone apoptosis after alpha and gamma irradiation, as measured by the flow-cytometrical annexin V assay. Globally, alpha radiation affected two-fold more genes than gamma. This was true for both cell types. Interestingly, there was little overlap between genes affected by both alpha and gamma radiation: 17% of genes in cells with mutated and 14% in cells with unmutated VH. Common genes were mainly involved in DNA repair: PCNA and CDKN1A acting in the p53-mediated pathway, CDC25B, CLK1 and CRY1. The 46 genes specifically altered by alpha exposure in mutated cells and the 33 genes in unmutated cells belong to a multitude of functional families, showing the generalized response induced including deregulation of cytokines, oncogenes, cell cycle regulating genes. Compared with alpha, effects of gamma radiation were of narrower range, with 24 genes altered in mutated and 16 in unmutated cells. Hierarchical cluster analysis after alpha and gamma radiation resulted in two clearly distinguishable array clusters, one grouping pts with mutated, the other pts with unmutated VH. In conclusion, transcriptional changes induced by alpha and gamma radiation encompass molecularly distinct mechanisms and reflect the higher complexity of DNA damage produced by alpha radiation. 121 Cyclotron production of Ac-225 for generating Bi-213 for targeted alpha therapy M.A. Chaudhri1,2, M.N. Chaidhri1, Q. Nadeem3, Q. Jabbar3 1Pakistan Council of Scientific and Industrial Research, Laboratories-Complex, Lahore, Pakistan, 2Institute of Medical Physics, Klinikum-Nuernberg,, Breslauer Str. 201, 90472 Nuernberg, Germany 3Department of Physics, Lahore College University for women, Lahore, Pakistan The generator system Ac-225 / Bi-213 (half life of 45,6 min) is a suitable method of producing an alpha-emitter for TAT. However, the production of Ac-225 is difficult and only a limited quantity of this isotope has so far been available for clinical use. Till recently it was exclusively produced by the decay of Th-229, which itself is

generated by the decay of U-233 (half life of 159200 years). By making use of our production yield curves we have estimated the production of Ac-225 through (p,2n) and (d,3n) on Ra-226, and also estimated the unwanted activities being produced simultaneously through (p,n), (d,n) and (d,2n) reactions on Ra-226. It is shown that from a thick Ra-target yields of 1.1 x 1010, 1.85 x 1010 and 2.04 x 1010 Bq respectively at proton bombarding energies of 20, 30 and 34 MeV can be obtained at incident proton current of 100 A but irradiation time of only one day which is a lot more practical than previously quoted 10 days. Similarly yields of Ac-225 through the (d,3n) reaction on Ra-226 have also been estimated to be 4.2 x 109, 1.1 x 1010 and 1.4 x 1010 Bq at deuteron energies of 20, 30 and 34 MeV respectively for irradiation time of 1 day at beam intensity of 100 A. As the yields data is presented in graphical form the production of Ac-225, from a moderately thick or even a thin Ra-226 target, can also be obtained for any irradiation conditions. Similarly, the unwanted activities through (p,n), (d,n) and (d,2n) reactions can also be estimated from the respective yield curves. 122 Whole body kinetics and dosimetry of 213Bi-labelled anti-CD20 based on pretherapeutic measurements with 111In-labelled anti-CD20 D. Schmidt1, F. Neumann2, C. Apostolidis3, S. Martin3, A. Morgenstern3, R. Molinet3, R. Kronenwett2, R. Haas2, H.W. Müller1 1University of Duesseldorf, Department of Nuclearmedicine, Düsseldorf, Germany 2University of Duesseldorf, Department of Haematology, Oncology and Clinical Immunology, Düsseldorf, Germany 3Institute for Transuranium Elements, Karlsruhe, Germany CD20-targeted radioimmuntherapy with alpha-emitting nuclides seems to be a promising new treatment for B-cell malignancies. In a first phase I dose escalation trial initiated to determine the safety and efficiency of 213Bi-labelled antiCD20 antibodies patients with relapsed or refractory non-Hodgkin´s lymphoma were treated (Heeger et al, 2001). Aim of this study was to get further data about biodistribution and pharmacokinetics of this tracer by pretherapeutical whole body measurements with 111In-labelled anti-CD20. Up to now in three patients dosimetry measurements using 111In-labelled anti-CD20 were performed to estimate the radiation absorbed dose to normal organs and bone marrow from 213Bi-Rituximab before therapy with 213Bi-labelled antibody. Planar anterior and posterior whole-body scans were acquired at 0.5, 2, 24 and 72 hours after tracer injection using a dual-head camera (Prism, Philips). In addition, in two patients images of liver and spleen were collected in dynamic mode during the first hour p.i.. The mean absorbed doses for various organs and the effective dose were calculated from geometric means of the anterior and posterior whole-body scans using ROI´s of the whole body and organs with tracer accumulation (liver, spleen, bone marrow). Uptake of 111In-labelled anti-CD20 in the bone marrow, liver, and spleen occurred within 5-min of administration and was maintained throughout more than 24 hours. No significant uptake was seen in any other organ, especially not in the urinary tract. Given the lack of significant excretion and the short half-life of 213Bi the whole body dose per amount injected activity was the same for each patient (0,00036 mGy/MBq). The absorbed dose delivered to the source organs is influenced by the extend of tumor infiltration and ranged from 3,3 - 7,2 mGy/MBq for the bone marrow, from 1,6 -1,7 mGy/MBq for the liver and from 2,4 - 6,1 mGy/MBq for the spleen. Depending on tumor burden the bone marrow seems to be the critical organ for therapy with Bi-213-antiCD20. However, it has to be taken into account that the reported mean absorbed dose to the bone marrow as well as to liver and spleen also contains the dose delivered for treatment.

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123 Target preparation method for irradiating Ra-226 in the Cyclotron at TUM and radiochemical procedures for extracting Ac-225 from irradiated targets J. Moreno Bermudez1, A. Türler1, R. Henkelmann1, E. Huenges2, E. Kabai1, G. Birebent1, M. Schilp3, M. Harfensteller3, A. Eursch3 1Technical University of Munich, Institute of Radiochemistry, Garching/Munich, Germany 2Technical University of Munich, Institute E17 of the Physics Dept., Garching/Munich, Germany 3Technical University of Munich, Institute for Machine Tools and Industrial Development, Garching/Munich, Germany Actinium-225 and its daughter isotope Bi-213 have been successfully used for immunotherapy in the treatment of specific types of cancer. One way for the production of Ac-225 is based on the proton irradiation of Ra-226 targets at a cyclotron using the nuclear reaction 226Ra (p,2n) 225Ac. In this work one of the methods developed for target preparation of Ra-226 is presented and discussed. This particular technique is based on the molecular electrodeposition of soluble Ra2+ from organic-aqueous solutions on aluminium cathodes of different geometries. This target preparation method satisfies the requirements imposed by the cylindrical geometry of the target designed for internal irradiation. We will also present and discuss the radiochemical procedures which were developed for the extraction of Ac-225 from the irradiated Ra-226/Al targets. These procedures are based on the selective leaching of both Ra and Ac from the irradiated Ra/Al targets and on the application of extraction chromatography materials (RE and Sr Resins) for the separation and purification of Ac from Ra and other important radioactive contaminants. The results obtained so far on the production yield of Ac, on the recovery factors and on the parameters of quality of the product (chemical and radioisotopic impurities measured in the Ac fraction) will be discussed. Scale test experiments with targets containing up to hundreds of micrograms of Ra-226 have demonstrated the feasibility of applying the electrodeposition technique for the irradiation of Ra/Al targets at the cyclotron and also the feasibility of extracting and purifying Ac from the irradiated targets by using the radiochemical procedures developed for this purpose. 123a Production of carrier free actinium-225/bismuth-213 and the application possibilities for alpha-immunotherapy C. Apostolidis, R. Molinet, A. Romanow, F. Bruchertseifer, A. Morgensten European Commission, JRC-ITU, Nuclear Chemistry, Karlsruhe, Germany For the selective irradiation of cancer cells, alpha-immunotherapy uses a-emitters such as Bi-213 and Ac-225 that are linked to monoclonal antibodies or peptides through bifunctional chelators. One production route via Th-229 has been further investigated, modified and improved. The carrier free Bi-213 is labelled to various monoclonal antibodies. For testing and application of alpha-immunotherapy, the regular supply of alpha-nuclides to hospitals that have embarked in pre-clinical and clinical trials is prerequisite. The poster will present the experiences with the separation processes, generator loading techniques and elution strategies as well as the overview on the different application possibilities of the ITU-produced Bi-213 in clinical trials. For the selective irradiation of cancer cells, alpha-immunotherapy uses a-emitters such as Bi-213 and Ac-225 that are linked to monoclonal antibodies or peptides through bifunctional chelators. One production route via Th-229 has been further investigated, modified and improved. The carrier free Bi-213 is labelled to various monoclonal antibodies. For testing and application of alpha-immunotherapy, the regular supply of alpha-nuclides to hospitals that have embarked in pre-clinical and clinical trials is prerequisite. The poster will present the experiences with the separation processes, generator loading techniques and elution strategies as well as the overview on the different application possibilities of the ITU-produced Bi-213 in clinical trials.

Track 5 – Session 4: PET Production & Application 124 Study of clinical application of 18F-FDG SPECT with coincidence in the recurrent or metastatic tumor of digestive system R.F. Wang, X.F. Yang, C.L. Zhang, F. Yan, Z.L. Fu, X.C. Zhang, Y.F. Wang, H. Tian, F.Q. Guo, G.Y. Zhao Peking University First Hospital, Nuclear Department, Beijing, China Purpose: To investigate the clinical value of 18F-FDG SPECT with coincidence in the diagnosis of recurrent or metastatic tumor of digestive system. Methods: 35 cases of postoperative patients with tumor of digestive system were enrolled in this study with 18F-FDG SPECT with coincidence. The results were analyzed by calculating its accuracy, sensitivity, specificity, positive predictive value (PPV), negative predictive value (NPV), and 95% confidence interval and compared with UB, CT and MRI. Results: In 35 cases of postoperative patients with tumor of digestive system, the accuracy, sensitivity, specificity, PPV and NPV were 91.4%, 88.9%, 100%, 100%, 72.7%, respectively, and their 95% confidence interval were 77% ~ 98%, 71% ~ 98%, 63% ~ 100%, 86% ~ 100%, 39% ~ 94%, respectively. The diagnostic accuracy and sensitivity of 18F-FDG SPECT with coincidence were significantly higher than that of UB, while there were no significant difference between the result of other 18F-FDG SPECT with coincidence and CT and MRI. The analysis of 95% confidence interval showed a higher tendency in 18F-FDG SPECT with coincidence than in UB, CT and MRI. There is complementation among 18F-FDG SPECT with coincidence combined with UB, CT and MRI in some cases. Conclusions: 18F-FDG SPECT/PET has high clinical value in the diagnosis of recurrent or metastatic tumor of digestive system. 125 Preliminary results of cancer screening with F-18 fluorodeoxyglucose positron emission tomography/computed tomography in Korea C. Kim, K. Lee, B. Kim, E. Kim RHRI, PET/CT Center, Seoul, Korea Objectives: primary cause of death is cancer in Korea and the only definite curative treatment is surgery, so early diagnosis of cancer is important. Our institute has been performing cancer screening with Positron Emission Tomography/Computed Tomography (PET/CT). We analyzed preliminary results of cancer screening with PET/CT over last 20 months. Methods: between February 2003 and September 2004, F-18 Fluorodeoxyglucose (FDG) PET/CET scan was performed in 2483 subjects who wanted cancer screening without previous cancer history (M:F 1336:1147, mean age 49.9 yr). Dual-modality PET-CT tomography, which is based on a dual-slice helical CT and a lutetium oxyorthosilicate (LSO)-based fullring PET tomography, was performed. PET/CT screening results were analyzed including further examination results for differential diagnosis in the view point of disease detection. Increased glucose metabolism findigns which did not mean malignancies were analyzed. Results: twenty cases were diagnosed as malignancies (0.8%); thyroid cancer 10 cases, colon cancer 4, lung cancer 2, gastric cancer 1, breast cancer 1, atypical malignant thymoma 1, renal cell cancer 1. In all cases surgical treatments were performed. Another twenty cases were diagnosed as precancerous lesions; colon adenomatous polyps (0.8%), and in all cases colonoscopic removals were performed. In benign disease thyroiditis (217 cases, 8.7%), thyroid nodules (218 cases, 5.2%), hepatic nodules (123 cases, 5.0%), renal cysts (18 cases, 0.7%) et al. were detected. In increased glucose metabolism findings which did not mean malignancies, focal bowel uptake and ovarian uptakes were observed frequently. Focal bowel uptakes were observed in 198 cases (8.0%). Analyzing 107 cases whose final diagnosis was concluded by PET/CT findigns or follow-up studies, 76 cases were concluded as normal (71%). Analyzing 267 women who had

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regular menstrual history, ovarian uptakes were observed in 98 cases (36.7%). Dates of their PET/CT examination ranged mainly in just or around ovulation or menstrual flow period. Conclusion: thyroid cancer, colon cancer, precancerous lesions were early detected on cancer screening with PET/CT with additional benign disease and curative treatments were performed. So, PET/CT examination is expected as one of the promising cancer screening examinations. However, focal bowel uptake on PET/CT needed careful interpretation and avoiding ovulation and menstrual flow period is recommended in pre-menopausal women. 126 Preparation of [61CU] Bleomycin complex as a possible PET radiopharmaceutical A.R. Jalilian1, P. Rowshanfarzad1, M. Sabet2, M. Kamali-dehghan, M. Mirzaii1, G. Raisali1, G. Aslani 1Cyclotron/Nucletron Medicine Department, Nuclear Research Center for Agriculture & Medicine, Karaj, Iran 2SSDL/Health Physics Department, Nuclear Research Center for Agriculture & Medicine, Karaj, Iran Copper-61 (T½=3.49 h) is an interesting radionuclide that has potential for positron emission tomography (PET) imaging of biological processes in intermediate to slow target tissue uptake. 61Cu was produced in the NRCAM cyclotron as a result of 15 MeV proton bombardment of nat.Zn with current intensity of 180 µA (yield 11.2 mCi/ µAh). Bleomycin (BLM) was labeled with [61Cu]CuCl3 for its possible diagnostic properties. The complex formation yield was optimized for pH, time, temperature, and ligand: radioactivity ratio. Radio-TLC showed an overall radiochemical yield of >98% (radiochemical purity 98%). The stability of the complex was checked in vitro. 127 11C-Methyl iodide production in a single use system F. Schmitz, E. Mulleneers, J. Van Naemen, B. Van Gansbeke, M. Monclus, M. Kadiata, S. Goldman ULB, PET/Biomedical Cyclotron Unit, Brussels, Belgium L-[S-11C-methyl]methionine is mainly used for brain tumours diagnostic1. Recently, Miterhauser et al2 have proposed to realize this synthesis in a single use system avoiding by this way the time consuming preparative HPLC. Their work as well as our previous experience3,4,5 could not get rid of the [11C-methyl]iodide production in a "classical" remote controlled system. We have focused our attention on the preparation of [11C-methyl]iodide in a full single use system expecting a more reproducible yield and avoiding a cleaning and sterilizing procedure. We are producing carbon-11 with the classical 14N(p,α)11C nuclear reaction: energy 16 MeV, pressure 30 bars, current 30 µA on a Cyclone-30 supplied by IBA. At the end of the bombardment, 11CO2 is extracted from the target and is directly trapped at -5°C in a solution of 1.0 M LiAlH4 in THF supplied by ABX (ref: 802.0001). After evaporation of the THF at 95 °C, HI (Aldrich, ref: 210013) is added, the system is completely closed and heated during 3 minutes at 105°C. [11C-methyl]iodide is distilled through KOH pellets (Merck, ref: 1604.0500) and trapped at -5°C in an ethanol solution (ref: 131780025). The complete process takes 10 minutes and a radiochemical yield EOB of (48±8) % (n=11) has been measured. The single use tubing is a slight adaptation of a valve rack supplied by GE for FDG synthesis with the Tracerlab MXfdg (ref: P 5150 ME). The specific activity of the final L-[S-11C-methyl]methionine has been measured higher than 1 Ci/µmole. With such a system, starting from 11CO2 produced in the target, we can synthesize L-[S-11C-methyl]methionine in a complete sterile single use system. 1. Becherer A., et al, Eur. J. Nucl. Med. Mol. Imaging, 30, 1561-1567 2. Miterhauser M., et al, Appl.Radiat.Isot., 62, 441-445. 3. Schmitz F., et al, J.Nucl.Med. 35, 82P. 4. Schmitz F., et al, Appl.Radiat.Isot., 46, 893-897. 5. Del Fiore G., et al, J.Labell. Compd. Radiopha

128 Recent activities on innovative radionuclide production for metabolic radiotherapy and PET and on relevant experimental and evaluated nuclear data C. Birattari2, M.L. Bonardi2, F. Groppi2, E. Menapace1, A. Martinotti2, S. Morzenti2, C. Zona2, L. Canella2 1ENEA, Division for Advanced Physical Technologies, Bologna, Italy 2Università degli Studi di Milano and INFN-Milano, LASA, Radiochemistry Laboratory, Milano, Italy Activities and relevant results are reviewed concerning the radionuclide production for medical applications brought up at LASA-INFN Laboratory, by collaboration with Cyclotron Laboratory of JRC-Ispra (EC) referring to irradiation experiments at K=38 variable energy Cyclotron. Mainly scientific aspects and applications have been investigated in order to obtain high specific activity accelerator-produced radionuclides in no-carrier-added (NCA) form. To this aim it was necessary to optimise the irradiation parameters, determining the excitation functions of the involved nuclear reactions, and to point out selective radiochemical separations of the radioisotopes of interest. The spectrometry measurements have been done at LASA-INFN: the γ, X spectra are measured with coaxial HPGe detectors, the spectra with Si surface barrier or PIPS detectors, with a resolution of 27 keV (FWHM), and spectra with a conventional liquid scintillation counting LSC and spectrometry system with Horrocks number capability and an higher-resolution liquid scintillation portable spectrometer with / pulse shape analysis (PSA) discriminator. Measurements of radionuclidic, radiochemical and chemical purities, by analytical and radioanalytical techniques, are discussed. Concerning the relevant excitation functions, evaluated nuclear data are discussed as they have been produced in collaboration with ENEA, Division for Advanced Physical Technologies, through appropriate comparisons of present and other available and critically selected experimental values with most reliable model calculations. The following NCA radionuclides, for uses in metabolic radiotherapy and PET, have been investigated: 1. NCA 64Cu, produced by natZn(d, xn) and natZn(d,2pxn) reactions for simultaneous β+/β- metabolic radiotherapy and PET, together with the short-lived radionuclide for PET imaging 61Cu; 2. NCA 66Ga, high-energy β+ emitter (4.2 MeV) for metabolic radiotherapy and PET; 3. 186gRe, produced by 186W(p,n) and 186W(d,2n) reactions for bone metastases pain palliation by β-(1.1 MeV) metabolic radiotherapy and SPECT imaging; 4. NCA 211At/211gPo, produced by 209Bi(α, 2n) reaction, with internal spike of emitter 210At from 209Bi(α,3n) reaction, for high-LET radiotherapy and immunoradiotherapy; 5. NCA 225Ac///213Bi/213Po, in-vivo nano-generator for high-LET radiotherapy and immunoradiotherapy. Main references are done to the international co-operation aspects particularly concerning nuclear data. 129 Need for innovative positron-emitting radionuclides for labeling of monoclonal antibodies (immuno-PET) L. Ferrer1, F. Haddad2 1René Gauducheau Cancer Center, Medical Physics, St. Herblain, France 2Subatech Laboratory, Nantes, France The recent development of 18F-Fluoro-deoxyglucose (FDG) and Positron Emission Tomography (PET) imaging has been a breakthrough in the field of cancer diagnosis. However the short physical half-life of fluorine-18 (110 min) is not appropriate to the slow kinetics of large antibody molecules. These molecules have a restricted specificity to some tumor types and can be used in clinical indications not properly covered by FDG. Consequently there is a need for antibody labeling by alternative positron-emitting radionuclides with longer half-lives than fluorine-18 and matched up to biological kinetics of various formats of antibody molecules (between 10 and 150 hours). The selection of these radionuclides should take into consideration various parameters such as technical characteristics of production (target enrichment, non radioactive targets, maximal cross section > 100 mbarns) which could have an impact on production cost. The

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physical characteristics of considered radionuclides (branching ratio >10%, maximal energy of positrons < 2 MeV, abundance and energy of associated gamma rays) could have an impact on imaging quality and patient and medical staff radioprotection. Based on these criteria, 16 positron-emitting radionuclides fulfilled the predefined conditions. The final selection of the radionuclides which will be produced by the high energy cyclotron planned in Nantes, France (protons, alpha particles 70 MeV, 350 mA) will be the optimal compromise between favorable and un favorable criteria. 130 Automated on-line preparation of [11C]-B-CFT, a dopamine transporter imaging agent J. Zhang1, J.H. Tian1, Z. Guo1, W. Ding1, S. Yao1, D. Yin1, B. Liu1 1The PLA General Hospital, PET Center, Beijing, China 2Beijing Normal University, Department of Chemistry, Beijing, China Objective: to develop an automatic synthesis method for the on-line preparation of dopamine transport imaging agent [11C]-b-CFT. Materials and methods: a mid-product, [11C]-methyl triflate made from [11C] methyl iodide, was bubbled into 0.1mg precursor nor-b-CFT at 5°C, to get [11C]-b-CFT. The final product, [11C]-b-CFT, was then purified though C-18 column eluted by 10 ml water twice followed by ethanol. The bio-distribution of [11C]-b-CFT was studied in SD rats. The human images were obtained in 6 cases of PD, and the results were compared with that of [11C]-Raclopride imaging. Results: the whole synthesis took about 4 min from [11C] methyl iodide to [11C]-b-CFT. The synthesis yield (EOB) was 92.4±3.1%, the radiochemical purity over 98%, and the specific activity about 2000Bq/mmol. [11C]-b-CFT were mainly concentrated in the liver, kidney and brain in SD rats. High uptake in striatum was noticed in brain. The uptake ratios of striatum to cerebellum were 2.15, 4.18, 3.15 at 5, 15 and 30 min after injection. [11C]-b-CFT was found more sensitive than [11C]-Raclopride in the early diagnosis of PD. Conclusions: the automated on-line preparation method was verified in producing [11C]-b-CFT of high radiochemical purity and synthesis yield in a short time. The products could be used in clinical imaging. Track 6: Education and regulatory aspects 131 Current status of licensing examination system in Korea K. Cho1, K. Chang2 1Korea Institute of Nuclear Safety, Department of Radiation Safety Research, Yusong, Taejon, Korea 2Ministry of Science and Technology, Radiation Safety, Seoul, Korea Korea has a constantly growing nuclear power program and radiation and radioisotopes industry. Especially, the number of licensed facilities for the use of radioisotopes and radiation generators has increased at an annual rate of 10 to 15% during the last three decades. There are more than 2,000 institutions in Korea, which use radioisotopes and radiation generators for medical, research and industrial applications. The Korean regulatory system for radiation protection related to the use of radioisotopes is based on the Atomic Energy Law, which stipulates the basic principles of radiation protection and peaceful application of atomic energy. The Law could be interpreted that the balance should be maintained between the promotion of the peaceful uses of atomic energy and radioisotopes and the safety regulation for securing the radiation safety. Current radiation protection laws and regulations of Korea are largely based on the international safety norms of the ICRP and IAEA. The license examination system, which has been implemented since the early 1960's, is a part of the Atomic Energy Law and is composed of three categories, namely general license, supervisory license and special license. Radioisotopes users should employ one type of license holder among the three kinds of licenses depending on their magnitude of the radiation risk associated with

their facility. This current license examination system is under review and is about to be revised in the first half of 2005 for the better management and control of radiation safety through the improved job assignment of license holders. 132 Safety regulations on production of radioisotopes in Korea W.K. Cho, K.H. Kim, B.H. Lee, K.H. Jeon, I.Y. Jeon, Y.J. Kim Korea Institute of Nuclear Safety (KINS), Radioactive Material Regulation, Daejeon, Korea Various kinds of radioisotopes for industrial, medical and research applications are being produced with a research reactor, HANARO and many cyclotrons in Korea. Radioisotope production is a practice involving with higher radioactivity or dose rates defined by the Enforcement Regulation of the Korean Atomic Energy Act. A person who intends to produce radioisotopes should obtain a license from Korean government. Safety regulatory organizations concerning radioisotope production are the Ministry of Science and Technology (MOST) as regulatory authority and the Korea Institute of Nuclear Safety (KINS) as a safety regulatory expert body. The safety in the production of radioisotope is being improved by multiple steps of regulation such as careful reviews in licensing, safety inspections for production facilities and products and periodic inspection on production status. All of safety reviews and inspections are performed by KINS on behalf of MOST. KINS assesses various types of application documents, such as safety analysis report, quality assurance program, and other documents evidencing fulfillment of requirements for license, submitted by a legal person who intends to produce radioisotopes and then reports the assessment result to MOST. A license for radioisotope production is issued to the applicant by MOST on the basis of a technical appraisal presented by KINS. A licensed manufacturer of radioisotopes should undergo facility inspections when he installs or alters the production facilities. A licensee also should undergo production inspection for radioisotope products by nuclear species and quantity when he produce radioisotopes for the first time or alter important characteristics of the radioisotope products. Radioisotope products to be inspected are categorized as sealed radioisotopes, unsealed radioisotopes and special form radioactive materials. In addition to the safety inspections for production facilities and products, a licensed manufacturer of radioisotopes should undergo periodic inspections annually on the production facilities and their operation status. A licensee also should report its production and sales status and inventory quarterly. 133 Training of Finnish radiochemists in the field of production of short-lived nuclides of transuranium elements K. Helariutta1, E.A. Gromova2, V.A. Jakovlev2, J. Aaltonen1, H. Ervanne1, A. Lunden1, A. Makkonen-Craig1, O. Perhola1, S. Salminen1, H. Tuovinen1 1Laboratory of Radiochemistry, Department of Chemistry, University of Helsinki, Finland 2V.G. Khlopin Radium Institute, Laboratory of Nuclear Reactions and Nuclear Meicine, St. Petersburg, Russia Important fields of research in the Laboratory of Radiochemistry, University of Helsinki (HYRL), are environmental radiochemistry and management and final disposal of radioactive waste. Short-lived transuranium nuclides, like 235Np and 236Pu are often needed as tracers in these kinds of studies but their commemrcial availability is limited. We have produced these nuclides previously by irradiating uranium targets with the K130 cyclotron of University of Jyväskylä, Finland, and the MGC-20 cyclotron of Abo Academic University, Finland. The radiochemical treatments of the irradiated targets have been made in HYRL the by a small group of senior scientists. HYRL has a compact IBA Cyclone 10/5 cyclotron, which was commissioned in 1998. Since then it has mainly been used for production of 18F for radiopharmaceutical syntheses, for research and clinical applications. Cyclone 10/5 is able to provide high-intensity proton and deuteron beams with energies of 10 MeV and 5 MeV, respectively. In order to take advantage of our cyclotron in teaching of radiochemistry, as well as to explore the possibilities of actinide tracer production with it, a

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practical course on isotope production was arranged in HYRL in August 2004. In this course the senior scientists from collaborating institute in Russia were teaching a group of radiochemistry students rangign from undergraduates to post docs. The course consisted a set of lectures on nuclear reactions, reaction cross section calculations, target preparation and methods of chemical separations of actinide elements. In the practical part a stack of thin 236U targets and A1 degrader foils were irradiated with 10 MeV protons. The targets were cooled and then measured by using alpha and gamma spectrometric methods. Different fractions from the separations were measured with alpha and gamma spectrometers. Based on the measurements, the students calculated chemical yields of neptunium and plutonium, as well as fusion reaction criss sections of 236,238U (p,xn) reactions. They completed their work by writing a report on the methods and results. Despite of the low incident proton energies, from 5 to 9.8 MeV, measurable amounts of Pu and Np isotopes were produced. The (p,n) cross sections are high enough to produce useful amounts of Pu tracers with our cyclotron in a 24-hour irradiation when uranium target of suitable thickness is chosen. 134 An overview of the design, testing, licensing and tracking of type B(U) containers at NTP radioisotopes PTY Ltd J. Selome1, M.E. Smith2, A.J. Bekker3 1NTP Radioisotopes, NECSA, Projects, Pretoria, South Africa 2NTP Radioisotopes, NECSA, Technology Development, Pretoria, South Africa 3NTP Radioisotopes, NECSA, Commercial, Pretoria, South Africa NTP ships products to approximately 40 different countries spread through five continents! One of the most important measures of quality in our sector (nuclear products) is dependability and reliability of supply, and suitably licensed containers play a significant role in complying with these requirements. Transport containers form an important part of NTP's value chain. The paper shares information on the stages followed in the development of transport containers, from the conceptual design, technical feasibility analysis, manufacturing of prototypes, testing, licensing and the subsequent tracking of fully licensed and endorsed containers using an in-house developed software system. At the end, challenges facing the entire Nuclear Industry regarding the safe transportation of isotopes are summarised. The Objectives: - To share NTP's experiences regarding the design, licensing, and tracking of Type B(U) containers, using the Beatrice Transport Package as an example. - To highlight the challenges facing the entire Industry, namely, successful shipping of isotopes in the midst of ever-tightening regulations of transport containers, and the threat posed by terrorism! 135 More than 40 years teaching radioisotopes techniques at the school of pharmacy and biochemistry of the Buenos Aires University, Argentina M. Zubillaga, G. Cremaschi, C. Davio, G. Cricco, G. Martin, A. Gutierrez, C. Cocca, C. Goldman, A. Klecha, A. Genaro, A. Bianchin, N. Mohamed, M. Salgueiro, G. Calmanovici, M. Nuñez, V. Medina, E. Rivera, R. Bergoc School of Pharmacy and Biochemistry. University of, Radioisotopes Laboratory. Physics Department, Buenos Aires, Argentina Ionizing radiation and radioisotopes are currently used in science and technology giving a great contribution to the improvement of our life and welfare. Some of the fields in which radioactive sources have been used during the last 60 years are: biology, biochemistry, medicine and pharmacology. The wildly spread use of ionizing radiation and radioisotopes in Argentina takes place at more than 1700 facilities, which operate in Nuclear Medicine (99Mo-99mTc columns, 131I), telecobalt therapy, Industry (60Co, 137Cs), biochemistry (125I, 32P) and research (99Mo-99mTc, 125I, 32P, others). All these centers have professionals trained in the field of radioprotection and they have been authorized by the Nuclear Regulatory Authority. At the School of Pharmacy and Biochemistry

of the Buenos Aires University, Argentina, we teach radioisotopes methodology at different levels, to harmonize the use of these methodologies with environmental preservation and to provide education and training on radioprotection. Currently, the School offers six different courses: 1. Methodology of Radioisotopes for undergraduate students in the Biochemistry Career (140 hrs), which gives them the guidelines for the adequate application and management of radioactive materials for their future work. 2. Methodology of Radioisotopes for post-graduates in Biochemistry, Biology, Chemistry or other related disciplines. 3. Course for Graduates in Medicine. Their syllabus (222 hrs) includes basic knowledge on radioisotope techniques, radiodosimetry, radioactive waste management and regulations. 4. Up-date on Methodology of Radioisotopes (100 hrs) for professionals wishing to up-date their knowledge specially on radioprotection aspects. 5. Course for Technicians in Nuclear Medicine (200 hrs), which mainly emphasizes the operational aspects of radioprotection at technician level. 6. Radiopharmacy, for undergraduate students in the Pharmacy Career (226 hrs). The goal of this course is to train Pharmacists in the preparation and quality control of radiopharmaceuticals for industry and radiopharmacies. The experience in research and teaching of more than 40 years in our Laboratory contributes to the professional and technical formation of the experts. We have a staff of more than 20 scientists and professors, most of them with the maximum academic degree (Ph.D.) and the participation of specialists from the National Nuclear Regulatory Authority, the Nuclear Medicine Services, and others. 136 A short historical overview of radiation dosimetry in medical exposure R. Van Loon1, R. Van Tiggelen2 1Vrije Universiteit Brussel, ELEC, Brussels, Belgium 2Belgian Museum of Radiology, Brussels, Belgium The measurement of radiation, quantitatively and qualitatively, has been an important task for physicians and physicists throughout the years. In early X-ray examination, the radiographer used his own hand, viewed in a fluoroscope, as a "penetrometer" in order to gauge the exposure required to x-ray the patient. In this contribution we will browse throughout history, to show the evolution of the assessment of quality and quantity of the radiation in medical exposure, based mainly on objects and literature on display in the Belgian Museum of Radiology, Brussels. The quality of the radiation was indirectly by absorption measurements or by measurement of the potential applied to the tube and directly, by measuring the wavelength of the spectrum components. We will introduce and illustrate several methods such as the "radiochromometer" of Benoist and the "skiameter" (in 1898), both based on absorption; the "spintermeter" already in 1900 where the X-ray tube potential was estimated by means of a spark-gap. The quantity was first related to tube current; then chemical methods such as the "chromoradiometer" of Holzknecht, and of Bordier and the "radiometer" of Sabouraud and Noiré appeared. Briefly mentioning exotic means such as measuring the heat produced by the tube, we will cover successively methods based on fluorescence, selenium conductivity, thermoluminescence and finally ionometric methods, leading to several different units such as the German R equal to 2.25 French R.. Clearly in the period extending from 1898 to the 1920s the basic principles still used for radiotion dosimetry were established and the scientists showed not only there inventiveness, but also their concern of beauty of the instruments. 137 August 2005: fiftieth anniversary of the first UN "Geneva Conference" Z.I. Kolar Radiation and Isotopes for Health Section, Department of Radiation, Radionuclides & Reactors, Faculty of Applied Sciences, Delft University of Technology, The Netherlands In December 1953 USA President D. Eisenhower held his “”Atoms for Peace"speech” before United Nations (UN) General Assembly

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which eventually led to the formation of the International Atomic Energy Agency (IAEA) in 1957. The advent of the IAEA was preceded by the first UN International Conference on the Peaceful Uses of the Atomic Energy, held in Geneva from 8 to 20 August 1955 which was attended by almost 2800 persons; both delegates and observers from 73 states! The Proceedings of the Conference containing all the papers and discussions of the Conference were published in 1956 in 16 volumes; each volume covering a main subject and its sub-subjects. Most of the papers dealt with physical and chemical aspects of nuclear reactors but also presented were papers on a number of other subjects, namely Radioactive Isotopes and Nuclear Radiations in Medicine, Biological Effects of Radiation, Radioactive Isotopes and Ionizing Radiations in Agriculture, Physiology, and Biochemistry, General Aspects of the Use of Radioactive Isotopes: Dosimetry and Applications of Radioactive Isotopes and Fission Products in Research and Industry. It is worthy to note that almost all abovementioned subjects are still of topical interest and appear in the "List of topics" of various conferences including the International Conferences on Isotopes (e.g. 5ICI). The first "Geneva Conference" was a remarkable gathering and that not only because of the great amount of information which was made public but also because of the expressed hope that the published proceedings will enhance the worldwide collaboration between the scientists and this all "for good of mankind"; a whish similar to the theme of the 5ICI, namely "Isotopes for Society". Although, it is not sure whether these expectations have actually been fulfilled as yet this should not prevent us to pay tribute to the participants of the first "Geneva Conference" held in August 1955 and celebrate the Conference's fiftieth anniversary.

5ICI 42 Poster Session I – Production and Transmutation

Posters (T1/S2) 138 New concept of 188W/188Re Generator with fully automated reconcentration Plat-form B. Lambert1, C. Gilles1, B. David1, F. De Vos2, H. Thierens3, G. Slegers4 1National Institute for Radioelements (IRE), Fleurus,Belgium 2Nuclear Medicine, Gent University Hospital, Gent, Belgium 3Medical Physics, Gent University Hospital, Gent, Belgium 4Radiopharmacy, Gent University Hospital, Gent, Belgium 188Re is one of the most promising isotope in the field of therapeutic nuclear medicine and can be easily obtained by elution of 188W/188Re generator system. The increased clinical use of 188Re for radiolabelling applications requires multi-curie quantities of 188Re with high radioactive concentration at reasonable cost. Additionally the elution process must be carried out in accordance with the GMP's. We have developed an alumina-based generator 188W/188Re in a highly shielded container in order to improve radiation protection for technicians. This new design allows to reduce whole body radiation dose at lower than 1µSv/elution. The elution can be realized with or without reconcentration and is monitored in real-time by fully automated plat-form with protected recording of critical parameters. The concentration of perrhenate (188ReO4

-) is based on tandem columns (Ag+-loaded strong cationic exchanger and anionic exchanger) included in a single-use disposable kit to ensure a sterile and pyrogen-free solution. The concentration units can overcome the drawbacks of using 188W with lower specific activity and allow the use of 188W coming from a larger number of nuclear reactors. In the frame of a cooperation agreement between the Gent University Hospital and IRE, four generators (from 27 GBq to 63 GBq of loaded 188W) were eluted two times a week over a period of three to four months with a reconcentration to a final volume of 5 ml. The average elution yield is around 75 %, the radionuclide purity greater than 99 %. All solutions are sterile and pyrogen-free. Furthermore the new radiopharmaceutical production line currently under construction at IRE for the manufacturing of 188W/188Re generators will be shortly described. 139 Absorption of radioiodine onto a platinum column M.M. Phetoe1, P. Mitchell1, J.R. Zeevaart2 1Necsa, Radiochemistry, Pretoria, South Africa 2Necsa, Nuclear Technology - Radiochemistry, Pretoria, South Africa Radioiodine (131I) is a very important radiochemical and it is used in the preparation of numerous radiopharma-ceuticles. Usually ion-exchange chromatographic methods and distillation are utilised for separation and purification of this particular radionuclide. There is a demand for higher purity of 131I. The new mechanism [1], aimed at producing pure and concentrated radioiodine, employs platinum powder (200 mesh) to adsorb iodine in acidic conditions. Adsorption and desorption processes take place on a panel, which is designed for liquids to be transported through the system by gases (hydrogen and argon). Adsorption is integrated on a vertical movement of trace solution on a reduced platinum surface. Desorption is performed electrochemically in alternation hydrogen and alkaline eluent. The benefits of this process are that the platinum column can be activated or regenerated for prolonged use, it is outstanding for optimising radioiodine, and it can purify 131I both radiochemically and chemically at the same time. The platinum column method is experimentally proven to have an efficiency of 99.6 ± 0.4%.

140 Radiochemical purity determination of I-131: comparison of a high-pressure liquid chromatography (HPLC) method with an alternative method S.C. Olsen NECSA, RadioAnalysis, Pretoria, South Africa The radiochemical purity of I-131 is of critical importance in the labelling of I-131 compounds as well as in the control of the total radiological dose received by patients who have been administered with I-131. Strict control of the radiochemical purity of the radioisotope I-131 is therefor necessary. Radiochemical purity is defined as the fraction of radioisotope that is in a specified chemical form. For I-131, that chemical form is the iodide (I-). Iodide is an unstable species and is prone to oxidation to the iodate (IO3-) form. Because of this (131I)Iodide is usually stored in alkaline solution, and may or not have added stabiliser. Other oxidative species of iodine that may occur include iodine (I2), hypoiodite (IO-) and periodate (IO4-). Historically, paper chromatography was the technique of choice in the determination of the radiochemical purity of I-131. Disadvantages of this technique include the loss of volatile species, air oxidation during spotting, and difficulties in quantification. A method for the determination of the radiochemical purity of I-131 was developed based on the separation of iodine-131 species on a silica gel column. The advantages of this method will be discussed and results will be compared to those of a standard HPLC method. 141 A fast way of determination of 202Tl impurity in 201Tl A. Sattari, N. Shadanpour, K. Kamali Moghadam, G. Aslani Nuclear Research Center for Agriculture and Medicin, Cyclotron and Nuclear Medicine, Karaj, Iran Introduction: in production of 201Tl by cyclotron, the long-lived 202Tl and short-lived 200Tl are usually present as impurity. In routine radionuclidic quality control, a sample containing 20-100 µl of thallium-201 solution in the final step of chemistry process is diluted and then detected by high pure germanium (HPGe) detector. This process takes about 1 hour and leads to significant absorption dose for technician who does this job. Material and methods: detection of 202Tl in a lead container has introduced by Bonardi (2001). We have developed the Bonardi's method, for detection of 201Tl using a HPGe detector with the 3 to 7 mm lead shields for the both aspects of quanity and quality. At first 201Tl purity was determined by usual method, later on we repeated measurement by using different thicknesses of lead shields. Results and discussion: comparing the results of two (new and routine) methods, correction coefficients for determinatino of real 201Tl and 202Tl impurity in the case of using lead shields were obtained. Errors related to dead-time, Compton continuum and X-ray fluorescence backgroun were very efficiently avoided and omitted. This rapid and simple method allows determinatino of 202Tl in 201Tl with sufficient accuracy in short time. In this method not only radiation exposure to the technicians reduced but also time of quality control process reduced to about 10 minutes in comparison with 1 hour for ruotine procedure. 142 Influence of the titanium molybdate preparation on the 99mTc generator performances based on gels F. Monroy-Guzman, J. Alanis-Morales, L. Galico-Cohen Instituto Nacional de Investigacioines Nucleares, Radioative Materials, Salazar, Mexico 99mTc is the most used radioisotope in Nuclear Medicine. It is produced commercially from 99Mo/99mTc generators where the 99Mo is adsorbed on alumina as 99Mo042- and 99mTcO4- is eluted from column with saline solution. This type of generators demands high specific activities of 99Mo which can only produce by irradiatino of 235U, originating a large amount of radioactive waste. Alternative generators constituted by molybdenum compound matrices open the possibility using lower specific activites of 99Mo, produced by the irradiation of stable 98Mo. This

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work proposes the utilisation of titanium molybdate gels as matrices of the 99Mo/99mTc generators. The preparation conditions of these gels influence directly on the generator performances, therefore, titanium molybdate gels were synthesized under different conditions, in order to establish the 99mTc generator performances and to choose the most appropriate gel to produce it commercially. In this case, the gels were prepared with no 99mTc followed by irradiation after their synthesis. Titanium molybdate gels were synthesized from TiCl3 and molybdate solutions varying the final pH of the titanium molybdate gels and the dissolution conditions of the TiCl3 solutions. These gels were then irradiated in the Triga Mark III Reactor (Mexico) and placed in glass columns in order to construct the 99mTc generator. The columns were then eluted over a period of one week every day and determined the generator efficiency and the radionuclide, radiochemical and chemical purity of the 99mTc eluates. A previous acid-base study of the gel is also shown. The variation of the gel pH has a well defined effect on the generator efficiency and the radiochemical purity of the 99mTc eluates. The efficiency decreases with an increase of the gel pH. In all the cases 99Mo breakthrough was less to 0.01. The best efficiency (~ 90%) was obtained in the gels prepared at pH around 5.9. 143 Role of redox-potential in the separation of Mo-99/Tc-99m in chromatographic systems L. Baranyai1, N. M. Nagy2, J. Konya2 1Institute of Isotopes Co., Ltd., Radiopharmaceutical Dep, Budapest, Hungary 2University of Debrecen, Faculty of Isotope Applications, Debrecen, Hungary Chromatographic separation of the 99mTc daughter element from its 99Mo mother one is based on the fact that in certain pH ranges oligomer ions are formed by assembling 7 to 8 individual ions which can be bound more strongly on the chromatographic column than single ions. However these oligomers form only in the highest oxidation state of the molybdenum. Consequently to seperate the daughter element from its mother one with high efficiency an appropriate redox-potential of the isotope mixture should be developed and maintained. At the same time in aqueous solutions with extremely high radioactivity, on the effect of radiolysis products, chemical reduction occurs which deteriorate the separation efficiency continuously. The actual separation efficiency is a function both of the oxidation (adding oxidation agent and/or bubbling air) and the counter effect, the radiolysis caused chemical reduction. The problem is even increased by the fact that the qualification procedure is extremely sensitive to the decrease in the separation efficiency already a very low decrease can cause unacceptable error in the yield. In our recent experiments redox-potential and its time dependence were investigated between platinum and calomel electrodes in solutions prepared in different way and conditions and the measured values were compared to the redox-potential of standard solutions. The oxidation agent concentration necessary to reach a good separation efficiency was determined and conclusions have been drawn for the decomposition rate of the oxidation agent. Impact of the redox-potential on the separation efficiency of Mo-99/Tc-99m chromatographic systems have been evaluated in respect of generator quality and generator yield. Posters (T1/S4) 144 Experimental demonstration of the new technology of medical Sr-89 production in solution reactor D. Chuvilin1, R.W. Brown2, V.E. Khvostionov3, L. Thome2, D.V. Markovskij4, V.A. Pavshook3, A.N. Udovenko1 1RRC "Kurchatov Institute", Institute of Molecular Physics, Moscow, Russia 2Technology Commercialization International, Albuquerque, USA 3RRC "Kurchatov Institute", Institute of Nuclear Reactors, Moscow, Russia 4RCC "Kurchatov Institute", Institute of Nuclear Fusion, Moscow, Russia

More than half of the world's annual production of radionuclides is used for medical purposes such as diagnostic imaging of diseases and patient therapy. 89Sr is used in nuclear medicine as a bone pain palliative agent for patients with bone metastasizes. Painful disseminated osseous metastases are common with carcinomas of the lung, prostate, and breast. The given report presents experimental demonstration of fragment 89Sr production in solution nuclear reactor by a principally new method, free of the traditional technologies disadvantages. The aggregate state of a fuel - aqueous solution of uranyl sulfate UO2SO4 - opens an unique opportunity to influence in a chain reaction not only a target radioisotope, but also its genetic precursors generated as a result of nuclear transmutations of fission fragments in a chain of decay of elements with the mass number 89: 89Se®89Br®89Kr®89Rb®89Sr. Krypton-89 - gaseous precursor of 89Sr has a life-time T½ =3.15 min sufficient for its escape from fuel solution into a gas phase. This process is based on "radiolytic boiling", starting from bubbles, containing water vapor and hydrogen-oxygen mixture, originated at fission fragment tracks. According to the experimental data, practically all long-lived isotopes of krypton and xenon leave in the gas phase of solution reactors. The report presents experimental studies of the mechanism of 89Kr transport in a solution reactor fuel, its cleaning from accompanying gaseous and volatile fission fragments, transportation of gas flow into the system of 89Kr retention, up to its complete decay into the target radionuclide 89Sr. The series of experiments are performed by taking the gas samples from the air cavity of the research solution mini-reactor ARGUS, operating at a power of 5-20 kW. The measurements are performed on determination of 90Sr content in a 89Sr chloride solution. It is demonstrated, that filtration of a gas flow by metal-ceramic filter and a solution cleaning with crown-ether Sr-Resin (for Strontium-specific) ensures reception of a 89Sr chloride solution of medical radionuclide purity. On the base of the received experimental data the productivity of the new technology was estimated as being approximately three orders of magnitude higher than for the traditional techniques used for commercial production of 89Sr. A solution reactor of 50-100 kW is capable of complete meeting the current demands in 89Sr in Russia with a sharp reduce of its production cost. 145 Phosphorus-32 production by sulfur irradiation in a partially moderated nuetron flux by 32-S(N,P) 32-P reaction J. Alanis1, J.M. Navarrete2 1Nuclear Center of Mexico, ININ, Ocoyoacac, Mexico 2Faculty of Chemistry, UNAM, Mexico Taking advantage of the fact that some positions for irradiation in the Mark III Nuclear Reactor of the Nuclear Centre of Mexico show neutron fluxes only partially moderated, phosphorus-32 has been produced by irradiating targets of previously purified commercial sulphur, by distillation at 444±2°C under nitrogen atmosphere, dilution of vapours in carbon disulphide, filtration of the solution through fibreglass, Teflon and cellulose, as well as final crystallization of Sα by CS2 evaporation. After irradiation during 6 to 20 hours with partially moderated neutron fluxes from 4.5 to 7.4 x 1012 n-cm-2-s-1, the sulphur target is distilled again at the same temperature, always under nitrogen atmosphere. Once the recipient made out from metal and Lucite is cooled, one oxygen flux is passed through during a few seconds, and the 32P is stuck on the recipient wall. When 25 to 50 ml of concentrated HCl are added, an acid solution of H3

32PO4 is formed. Once this acid solution is diluted and pH fixed to an adequate value, labelled ortophosphoric acid is available to obtain labelled phosphates to be used in biological and agricultural studies. Chemical and radiochemical purity of these substances are almost total. At this stage, till 12 mCi of H3

32PO4 have been obtained for a Sα target mass of 5 g. The procedure seems to be so reliable that industrial, periodical production is being planned to start in a few months.

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146 A new conceptual design of an irradiation capsule for 125I production in a reactor U. Park1, J.S. Lee1, K.J. Son1, H.S. Han1, H.I. Kim2, B.J. Jun2 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Daejeon, Korea 2Korea Atomic Energy Research Institute, HANARO Management Division, Daejeon, Korea A new capsule design is developed to produce high purity 125I by an irradiation of natural xenon gas. This capsule is a cylindrical type and consists of upper and lower parts. The lower part is immersed in the neutron flux zone, and the upper part serves as an absorption reservoir for the 125I produced from the activated 125Xe. To increase the absorptioin capacity of the upper part, vertical heat-exchange fins are attached to the outer surface of the upper part. A guide baffle is inserted along the center line to make the gas circulation between the upper and lower parts smoother. The conventional flow rate and temperature distribution inside of the capsule (1:30 cm, dia: 4.95 cm, t: 2mm) are computed by the CFX 4 code to evaluate whether there is a continuous circulation of the filled gas at 1.0 atm pressure. The computational results show that xenon gas circulates once every five seconds, and the temperature of the surface of the upper part is 77°C. The maximum temperature reaches 550°C at the center of the lower part. These results will be employed as basic data for future experiments. 147 Structural analysis of gas capsules for the production of 125I K.J. Son, U. Park, S. Nam, S. Hong, J. Park, H. Han Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Yuseong-Gu, Daejeon, Korea Various safety tests and structural analyses have been performed on the sealed capsules of an Xe gas target for the production of 125I. Since the target is a gas, the structural integrity and the leak tightness of the capsules are thoroughly examined. The capsule of the Xe gas target was designed as a double encapsulation so that no gases could escape during an irradiation. And it is fabricated with high purity aluminium (A1050) for minimizing radioactive waste and absorbin the gas of 125I. We estimated the heat generation during a neutron irradiation using the MCNP code and calculated the temperature distributions of the capsules by applying the results from the heat generation analysis. By using the FEM code, ABAQUS, we evaluated the mechanical strength of the capsules when they were exposed to irradiation conditions. Vacuum bubble leakage tests were also performed after heating the capsules at 400°C for 8 hours. From these analysis and tests results, we established the safety and integrity of the gas target capsule for the production of 125I. 148 Possible way to industrial production of Nickel-63 and the prospects of its use A.V. Tikhomirov1, L.A. Tsvetkov2, A.A. Pustovalov2, V.V. Gusev2, V.Y. Baranov1 1Russian Research Center "Kurchatov Institute", Moscow, Russia 2Research Industrial Enterprise "BIAPOS", Moscow, Russia Nickel-63 is a pure beta-ray emitter with a half-life of 100 years and a maximum beta-ray energy of 65 keV. This radioactive isotope could be used as a long-lived source of energy in various devices (implantable biostimulators, in electronic etc.) but the cost of the product is too high and the volume of production is very small. The reason is the accepted and so far single technology of nickel-63 production. This technology involves neutron irradiation of targets preliminarily enriched with nickel-62 as an original isotope. The desire to increase the specific activity leads to the highest enrichment of the targets and their irradiaton in ultrahigh-flux nuclear reactors. This is a rather expensive, but not effective, process, because the nuclear-physical characteristics of nickel do not allow one to reach a nickel-63 content of greater than 30% of the initial nickel-62 in the irradiated target. The real economic reasons restrict this figure to 15-17%. This report proposes an industrial method of producing the highly-enriched nickel-63 (with

a concentration of up to 80-90%) in kilogram amounts. The problem can be solved if the target nickel is charged into the channels of industrial and/or power reactors of the RBMK and ADE type with medium-level neutron fluxes. The inexpensive use of these reactors in comparison with ultrahigh-flux neutron sources allows a long-term campaign with a nickel charge of hundreds of kilograms. The centrifugal technologies that are widespread in Russia allow large-scale separation of natural nickel isotopes and production of targets enriched with nickel-62. In this case, the target nickel does not require a high enrichment with nickel-62. The degree of enrichment is chosen from the proper relation between expenditures on separation, neutron irradiaion and radiochemical conversion. Centrifugal separation could be also used to increase the specific activity of nickel-63 after irradiation. The well-adjusted production cycle can ensure the output of tens of kilograms of nickel-63 with a concentration of about 80%. It is important that such a production excludes the build-up of radioactive wastes. The nickel preparations with a nickel-63 concentration of 70-80% could expand the area of application of soft beta-ray emitters presenting no radiation problems. The basic task consists in the efficient and sufficient production of the nickel-63 radioisotope with a high specific activity. 149 Production logistics and prospects of 142Pr and 143Pr for radionuclide therapy (RNT) applications K.V. Vimalnath1, M.K. Das2, M. Venkatesh1, N. Ramamoorthy3 1Bhabha Atomic Research Centre, Radiopharmaceuticals, Mumbai, India 2Board of Radiation and Isotope Technology, Radiopharmaceuti-cals, Kolkata, India 3IAEA, Physical & Chemical Sciences (NAPC), Vienna, Austria Two radionuclides of praseodymium appear attractive for RNT applications. 142Pr decays by beta emission (Eβmax 2.16 MeV) with a half-life of 19.12 hours. It has a low intensity (3.7%) 1.575 MeV energy gamma emission. Praseodymium is a mono-nuclidic element (containing 100% 141Pr) and has a fair cross-section of ~ 11.5 barn for (n,γ) reaction. 142Pr was produced at the rate of 2.5 GBq per mg of Pr after 3-4 day irradiation at a thermal neutron flux of ~ 5x1013 n.cm-2.s-1. Traces of 153Sm, 140La were detected in the final product, but the RN purity of 142Pr was >99.97%, comparable to that of 153Sm viz.>99.8% specified in USP. In comparison to 1.3 barn cross-section for production of 90Y from 89Y target, 142Pr would thus be a better candidate of high energy beta emission and producible in a medium flux research reactor. 142Pr appears to be a suitable choice for therapies requiring higher rate of dose delivery, either alone or in combination with a longer half-life product for mixed radionuclide therapy. 143Pr (t½ 13.57 d and Eβmax 0.937 MeV) is beta decay product of 143Ce (t½ 33.04 h) and an ideal complement to the widely used 32P (t½ 14.3 d, Eβmax 1.71 MeV), for some applications in radionuclide therapy (RNT), as it has a lower beta energy, but comparable half-life. For the production of 143Pr, 10-500 mg of two cerium compounds, ceric ammonium sulphate and ceric oxide, were irradiated in the reactor for 7 days at a neutron flux of ~ 1x1013 n.cm-2.s-1. After five days of post irradiation cooling, the samples were dissolved in appropriate reagents and aliquots were subjected to high resolution gamma ray spectrometry for assay of activity and radionuclide purity. An effort was made for the separation of no-carrier added (nca) 143Pr in order to study its utility for radionuclide therapy (RNT). A maximum yield of ~ 450 MBq of 143Pr was obtained at calibration time defined as 7d from end of irradiatin (EOI). RN purity of 143Pr in the final product was more than 99.9% with Ce content less than 0.9ng. Despite the low cross-section of 142Ce(n,γ) reaction (0.1 barn) and 11.11% isotopic abundance of 142Ce in natural targets, therapies needing low to medium doses (such as radiation synovectomy of medium and small joints, sk, skin patches for treating superficial tumours) would benefit from the use of "nca" 143Pr.

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150 The use of isotope Se-74 for the production of the high specific activity radionuclide Se-75 and sources of ionizing radiations V.B. Bogod1, A.N. Cheltsov2, L.Y. Sosnin2, E.A. Zhukovsky2 1JSC "Energomontage International", Moscow, Russia 2RRC "Kurchatov Institute", Moscow, Russia Survey made at Russian Research Center "Kurchatov Institute" has shown the possibility to separate all Selenium isotopes on centrifuges using SeF6 as work substance. The difficulty to obtaine highly enriched 74Se is defined by its low natural content (C=0,87%). It is possible to obtaine radionuclide 75Se with high specific activity and radionuclide purity from highly enriched 74Se (C>96%) by raying it with neutrons. The radioactive 75Se are used in medicine, for research and as γ-emitter in portable flaw detectors for exposure to gamma-rays of pipe welds under field with high image sharpness at steel thickness up to 30 mm. Having half-life being 127 days selenium-75 after emission is converted into stable arsenic which rules out the emergence of ecological problems after operating time of the radioactive ampoule in flaw detector. The Selenium-75 gamma ray spectrum covers the energy range from 66 keV to 401 keV. Two lines of high intensity at 137 keV and 265 keV dominate the spectrum. The radiation characteristics are in between of Yb-169 towards lower and Ir-192 towards higher energies. This makes Se-75 the ideal choice for gamma radiography in the wall thicknees range of approximately 5 to 30 mm of steel. Se-75 provides significantly higher image quality than Ir-192. A gamma ray projector can be used in a large range of radiographic applications with a demand for high image quality. This includes the inspection of weldments on pipes, pressure vessels or other safety relevant parts. High image quality is one important technical aspect for the use of Se-75 Handiness and simplified radiation protection requirements plus a very favourable halflife of 118 days add enormous economical advantages. 151 Production of 188W at SSC RF RIAR using SM high-flux reactor R.A. Kuznetsov, V.A. Tarasov, S.I. Klimov, A.N. Pakhomov, O.V. Bubas Federal State Unitary Enterprise, State Scientific Center of Russian Federation, Research Institute of Atomic Reactors Russia Principal results of the RIAR technology development for production of tingsten-188 are reported. Problems of tungsten-188 production by irradiation in the SM research high-flux reactor as well as radiochemical processing of irradiated targets are discussed, estimated cross-sections of radionuclides of tungsten-188 production chain are given, and the technology flow-sheet developed by RIAR is briefly described including targets dissolution and purification of tungsten-188 from impurities. Based on results of experiments (samples irradiation in positions with considerably different neutron flux density and various neutron spectra) kinetics of 188W production was studied and a system allowing proper prediction of this radionuclide accumulation in the SM reactor was developed. It was demonstrated that thermal neutron flux density is the determining factor at reactor production of this radionuclide. Irradiation in hard or fast neutron spectra gives no rise in specific activity of 188W. Duration of continuous irradiation cycle is of high importance at 188W production as concentration of 188W nuclei follows concentration of short-lived predecessor - 187W; after each reactor shut-down or its power decrease the yield of 188W certainly drops down. Processing of irradiated tungsten targets includes conversion of the irradiated material to a solute state, purification from impurities, radioactive and non-radioactive ones, conditioning of the purified solution (adjusting of component concentration). After irradiation in the SM reactor during one reactor campaign more than 20% of 186W burns-out to 187Re. Thus, processing technology of irradiated targets (after their dissolution in basic solution containing sodium hypochlorite) includes anion-exchange purification from rhenium using Dowex-1 type anion-exchanger in nitrate-form. The second

processing stage is purification from silicon impurity which contaminates product at targets dissolution stage. This stage is performed by anion exchange chromatography using Dowex-1 type resin in Cl¯form. Besides, this stage allows for purification from anionic impurities that are products of destruction of oxidizing agent NaOCl added to a solution at targets dissolution stage (chloride, chlorate, perchlorate ions). The final stage is desalination of the solution (removal of an excess of sodium) which is performed by passing the solution through the column with the Dowex-50 type cation exchanger; tungsten is stabilized in the solution by adding hydrogen peroxide. The solution of pertungstic acid is evaporated to dryness producing tungstic acid which is dissolved in desired quantity of base. Total radioactive impurities content in the final product is not higher than 0.2-0.5%. 188W specific activity depends on irradiation terms and is regularly ~4.5 Ci/g. 152 Comparative evaluation of logistics of preparation and quality control (QC) testing aspects of 99mTc from different generator sources using (n,γ)99Mo N. Ramamoorthy1, P. Saraswathy2, S.K. Sarkar2, G. Arjun2, S. Chattopadhyay3, M.K. Das3 1IAEA, Physical & Chemical Sciences (NAPC), Vienna, Austria 2Board of Radiation & Isotope Technology, Radiopharmaceuticals, Navi Mumbai, India 3Board of Radiation and Isotope Technology, Radiopharmaceuti-cals, Kolkata, India 99mTc is commonly available by eluting alumina column pre-absorbed with 99O of high specific activity obtained by thermal neutron fission of 235U. An alternate 99mTc delivery system prepared from (n, γ) 99Mo of low/medium specific activity is the gel generator based on zirconium molybdate-99Mo (Zr99Mo) which would be of good utility if there is easy access to (n, γ)99Mo of specific activity 0.5-1Ci per g of Mo. Standardization of preparation and evaluation of utility of these generators have been successfully established although the process is demanding in terms of remote handling facilities for safe and reliable operations. The concept of post-elution concentration of perrhenate and pertechnetate mooted by the ORNL group gave a fillip to the prospects of using a jumbo (40-50g) alumina column generator loaded with (n,γ)99Mo. This is coupled to a small anion exchange column (DEAE cellulose, 600 mg) to trap the pertechnetate present in 60 ml of 1:1 v/v:: 0.05M NH4OAc: 0.7M HOAc eluate and increase the radioactive concentration by re-elution in small volume of normal saline to deliver 99mTc. In another method, the pertechnetate eluate in 70 ml normal saline was trapped on a tiny column of Dowex-1 x8 (10-15mg), re-eluted in 0.2M Nal solution and passed down a AgCl (1g) column to remove iodide as AgI and obtain pertechnetate in isotonic saline. The major merit of the second method is that, it functions (nearly) independent of the volume of the primary eluate from the alumina column and hence can be coupled to 80-100 g size column beds to deliver higher capacity generators. Another fruitful outcome achieved was in establishing the feasibility of dual purpose use of the secondary trap column of alumina in the Zr99Mo gel generators for purification-cum-concentration of pertechnetate after eluting the gel column with de-ionised water. This has widened the scope of utility of gel generator, even when faced with lower specific activities of 99Mo. The acceptance of the systems by the users would be dictated by the relative user-friendliness, safety and reliability of product quality, quantity and radioactive concentration of pertechnetate deliverable, ease and duration of operation and overall cost-effectiveness. Zr99Mo gel generator system along with the strategy to exploit the post-elution concentration appears to have an edge over the other systems.

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153 Production of Tc-99m generator using advanced manu-facturing facilities in Korea B.C. Shin1, W.M. Choung2, S.J. Kim2, S.M. Choi2, S.H. Park2, J.H. Park3, K.B. Park4, M.S. Kim5 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Daejeon, Korea 2Korea Atomic Energy Research Institute, Division of Spent Fuel Management Technology Research, Daejeon, Korea 3Korea Atomic Energy Research Institute, Division of Decommissioning Technology Development, Daejeon, Korea 4Korea Atomic Energy Research Institute, Center for HANARO Applications Research, Daejeon, Korea 5Sam Young Unitech Co., Ltd., Korea Technetium-99m is the most widely used radionuclide in clinical nuclear medicine for a diagnosis. For the characterization of radiopharmaceuticals, a manufacturing facility should be complied with the radiation safety standards for operators as well as the GMP (Good Manufacturing Practice) cleanness standards for the production system. We have intensively modified the existing Radioisotope production facilities, which were installed only from a radiation safety point of view, to meet the cleanness criteria. And the concept of multi-barrier buffer zones was introduced to apply a negative air pressure to the hot cell as a first priority and to maintain a relative positive air pressure for the clean room. Three lead hot cells were installed and a final inspection including a gamma survey test was performed. The clean room was installed and the TAB (testing, adjusting & balancing) for this facility was performed in order to acquire the necessary air flow. A filter bank for the filtration of the exhaused radiation air was installed and its efficiency test was performed. In this facility, radiation shielding utilities and manufacturing instruments were set up and their operating manuals were documented. Efficiency tests for all the utilities and instruments were satisfied and an approval for the use of the facilities was achieved from MOST (Ministry of Science and Technology). Sam Young Unitech, the lessee of the facilities set up the manufacturing equipment for the Tc-99m Generator, supported by the IPPE in Russia. They improved its production process and modified a lead container more convenient and nicer than the original one. They obtained manufacturing license and production license from KFDA (Korea Food and Drug Administration) and have been producing the Tc-99m Generator with 200 to 1,500 mCi since July, 2004. KAERI assists in the quality assurance for the Tc-99m Generator. The labeling yield was shown at more than 98% with the cold kits such as MDP, DISIDA, DTPA, DMSA and MIBI. Posters (T1/S5) 154 Dependence of TEO2 recov ery on impurities nature in regeneration process B. Kudelin, L.M. Solin Radium Insitute, St. Petersburg, Russia Iodine-123 and iodine-124, widely used in nuclear medicine, can be effectively produced by irradiation of tellurium dioxide targets at low energy cyclotrons via p,n reaction. During the targets operation some part of isotopically enriched tellurium dioxide is transferred onto the inside surfaces of the used apparatus, such as target device and iodine sublimation apparatus. In order to return high expensive enriched TeO2 material into the production process a target regeneration procedure has to be undertaken. The procedure includes recovery of dispersed tellurium dioxide and purification of the collected material by means of dry vacuum sublimation method which is the most convenient and fast way of TeO2 purification. Usually TeO2 before regeneration is contaminated by silica and some metal oxides. It has been found in our investigation that at high temperature the contaminations react with tellurium dioxide yielding nonvolatile tellurous acid salts. These compounds prevent TeO2 from full evaporation during the purification process,

decreasing the yield of regenerated tellurium dioxide. Quantities of tellurium fixed by different contaminations have been measured. Main functional changes of the targets during exploration are also discussed along with some ways of the targets life time prolongation. 155 Production of a prototype 68Ge/68 Ga generator B. Shirazi, B. Fateh, M. Mirzaii, G. Aslani Nuclear Research Center for Agriculture and Medicine, Atomic Energy Organization of Iran, Karaj – Iran Gallium-68 is a radioisotope with half life of 68 min and popularly used in nuclear medicine. The only way to obtain these nuclides is to produced the mother nuclease(Ge-68) and the best reaction is 69Ga(p,2n)68Ge. The cross section of this nuclear reaction was calculated and compared with the practical work done by other researchers. The comparing result was an acceptable one so, the best proton energy was calculated to be between 20-25 MeV. Further research showed that Ga2O3 is the best type of target material. Therefore suitable target holder (for the very first time in Iran) designed at Nuclear Research Center for Agriculture and Medicine (NRCAM). The thickness of the target, bearing in mind the rate of energy loss in side the target material, was calculated and the Ga2O3 tablets were made with FT-IR instruments. They were then bombarded with the 20, 21 and 22.5 MeV proton energy and the beam currents of 1.4, 7.5 and 13.3 µA. Two weeks after the bombardment the radio chemical separation of Ge-68 was done with concentrated acid HNO3 and applying heat. Then, the acid solution was evaporated till dried after that, an EDTA solution (0.005 M, pH = 11) was added to recover the Ge-68. By passing the EDTA solution through the Al2O3 column, Ge-68 radioisotope was adsorbed. Then another solution of EDTA(0.005 M, PH=11) was passed thorough the loaded column, almost all the natural Gallium impurities were removed. In this project the behavior of natural Gallium was studied via adding Ga-67 as a tracer which its half life is about 78 hours. Therefore the best flow rate and volume of the eluant within the loading and milking the generators were determined. The best flow rate of eluant and also best volume of the second EDTA solution to remove almost all the natural Gallium impurities were determined to be 0.5 mL/min and 50 mL. The prepared generators were milked many times with EDTA solution (0.005 M, PH=8) and the leakage of Ge-68 nuclease and natural Gallium were determined. The average of the mother nuclides (Ge-68) was about 0.03% and the natural Gallium was 0.7 µgr./Lit., which is compatible with other research reports. Attention on suitable results shows that radiochemical loading and milking yield were more than 69-75 percent respectively. Therefore if better target holder were designed, Ga2O3 targets can be bombarded with higher current, hence it is possible to improve the more powerful 68Ge/68Ga generato 156 Germanium-68 row of products A. Razbash1, N.N. Krasnov1, Y.G. Sevastianov1, A.I. Leonov2, V.E. Pavlikhin2 1Cyclotron Co. Ltd, Radiochemical Laboratory, Obninsk, Russia 2Cyclotron Co. Ltd, Sources Laboratory Radionuclide germanium-68 has half-life of 270.8 days and decays by electron capture into gallium-68. The daughter radionuclide has relatively short half-life of 68 min and is a positron emitter. Germanium-68 is in equlibrium with gallium-68. And the wide application of germanium-68 is connected just with gallium-68. A series of products with germanium-68 begins from germanium-68 as a radiochemicals. It is the first step to provide different applications with Ge-68 as a row material. The developed separation technique allowes to produce germanium-68 with very high chemical and radiochemical purity. The specific activity is more than 2.5 Ci/mg and radionuclide purity is more than 99.8%. The main application of this radionuclide is positron emission tomography (PET). PET-devices are needed in sources for calibration or normalization. The original technology for line sources production, based on the electrodepositition of Ge-68 on a

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copper wire, ensures uniformity of Ge-68 distribution and allowes to get line souces with desired length, in other words for a use in PET-devices of any producers. Line sources are produced with an activity of Ge-68 up to 20 mCi. Phantom sourse also serves calibration purpose. Both types of the sources have ISO-classification - C 22221. The next product of Ge-68 products is Ga-68 generator. The generators are produced with an Ge-68 activity up to 50 mCi. They allow to obtain Ga-68 in 0.1 M hydrochloric acid solution at any time you want. This solution can be used for a calibration of PET-system, for a making of different phantoms and for a development of labelling technique. The positron source based on Ge-68 is the last product in this row now. The production technology includes the electrodeposition of Ge-68 on the support and its follow-up hermetically closure in Ti-capsule. The window is made from thin Ti-foil. 157 Energy spectrum and dose distribution of neutrons and gamma rays in the labyrinth through the NRCAM Cyclone30 Shield G. Raisali1, N. Hajilo1, S. Hamidi2, G. Aslani1 1Atomic Energy Organization of Iran, Nuclear Researh Center for Agriculture and Medicine, Karaj, Iran 2Arak University, College of Sciences, Arak, Iran One of the isotopes produced in Nuclear Research Center for Agriculture and Medicine (NRCAM) is Thallium-201 via 203Tl (p, 3n) 201Pb reaction using cyclotron Cyclone30. Due to high intensity of the neutrons and gamma rays produced from the Tl target and its Copper substrate, a concrete shield with a multi-bend labyrinth is used for the target room. As it is planned to upgrade the cyclotron in NRCAM to higher intensities, a detailed study of the shield performance have been investigated in this work. In this article, neutron and gamma ray equivalent dose rates in various points of the maze are calculated by simulating the transport and streaming of neutrons, and photons using Monte Carlo method. For determination of neutron and gamma ray source intensities and their energy spectrum, we have applied SRIM and ALICE computer codes to Tl target and its Cu substrate for 145 mA of 28.5 MeV proton beam. The MCNP code has been applied with neutron source term in mode n p to consider both prompt neutrons and secondary capture gamma rays. Then the code is applied for the prompt gamma rays as the source term. By defining the shield geometry of the target room, the streaming of the radiation through the labyrinth is simulated. For speeding up the calculations, splitting and Russian roulette variance reduction techniques have been applied by a very efficient consideration and application of importance concept. The neutron and gamma ray production rates have been calculated as 1.22E13 n/s and 1.96E13 gamma/s respectively. The neutron flux energy spectrum and equivalent dose rates for neutron and gamma rays in various positions in the maze have been also calculated. The calculated dose rates are compared with values measured by Berthold LB 6411 neutron dosimeter, and a gamma dosimeter calibrated in NRCAM SSDL laboratory. It has been found that the maximum deviation between calculated and measured values occurs at the farthest position from the source, namely at the entrance door of the maze, for which neutron and gamma equivalent dose rates have been calculated as 0.109 and 0.047 mSv/hr, respectively. The corrected measured neutron dose rate values, based on MCNP calculated energy spectrum, and the gamma dose rate at the entrance position have been measured as 0.136 and 0.057 mSv/hr respectively. At other points in the labyrinth, the average difference between the calculated and measured dose rate value have been less than 25%. 158 Solvent-solvent extraction of carrier free 103Pd from the Rhodium irradiated by the a-furyldioxime M. Sadeghi1, B. Shirazi2, H. Afarideh2 1Research and Science Campus, Islamic Azad University, Faculty of Engineering, Tehran, Iran 2Nuclear Research Center for Agriculture & Medicine, Cyclotron Department Karaj, Iran

The separation of 103Pd formed in rhodium target by irradiation with 18 MeV protons or deuterons is a rather difficult problem. The first problem is the dissolution of rhodium metal and the second one is the high quantity of rhodium in solution. For the separation of small quantities of palladium from an excess of rhodium the most suitable is the extraction method. There are many extractants for palladium used mainly in analytical chemistry. The best known dimethylglyoxime was used for the separation of 103pd from rhodium, but we experienced that with increasing quantity of rhodium the yield decreased, more suitable is α-furyldioxime. This extractant gives with palladium a stable complex. Palladium is selectively extracted from acidic solution into chloroform. Owing to the great quantity of rhodium in solution, chromatographic separation methods successfully used for the separation of comparable quantities of palladium and rhodium do not give good results. Fragments of irradiated rhodium were prepared by dissolution of copper carriers of electroplated Rh targets in concentrated nitric acid. The dissolution of rhodium fragments was done in a cylindrical vessel with two graphite electrodes by applying alternating current up to 30 A and hydrochloric acid with concentrations of 6 and 12 N. The solution was evaporated nearly to dryness. The residue was dissolved in distilled water /acidity of the resultant solution of 0.7 g rhodium. To the rhodium/103Pd solution in HCl, a 1 ml alcoholic solution of 5 mg α-furyldioxime and 39 ml chloroform were added. The mixture was vigorously stirred for 10 min. After separation of the organic layer, the organic phase was washed with 0.6 M HCl. Then aqua regia (10-15 ml) was added to this phase, and the mixture was evaporated to dryness on an electric heater. The residue was treated with a fresh solution of aqua regia and hydrogen peroxide, and the resulting solution was evaporated. After complete degradation of organic compounds, the residue was twice evaporated with hydrochloric acid to wet salts to remove residual oxidizing agents and to convert 103Pd into the chloride form. The final product was dissolved in hydrochloric acid of the desired concentration. Radioactivity of 103Pd was measured on an HPGe detector and the extraction was repeated several times. Results are summarized in Table 1.

Acidity of HCl (N)

Distribution ratios Dv

Extraction %

0.2 0.37 0.7 1 4 7

2.35 5.8

1.577 1.29

0.772 0.62

70.1 85.3 61.2 56.3 43.6 38.3

159 Production and quality control of 61Cu radioisotope in a 30 MeV cyclotron P. Rowshanfarzad, M. Sabet, A.R. Jalilian, M. Kamalidehghan, M. Mirzaii Nuclear Research Center for Agriculture and Medici, Cyclotron and Nuclear Medicine, Karaj, Iran In this article, selection of production parameters for the production of 61Cu radioisotope in NRCAM cyclotron, including selection of the appropriate nuclear reaction, proton beam energy, target thickness and the targetry method are discussed. Due to the results of ALICE and SRIM nuclear codes, and analysis of the relevant data and assessment of the present conditions, 64Zn(p,α)61Cu was selected as the best reaction for the production of 61Cu. The optimum proton beam energy was 12-22 MeV and the best target was 80 microns of natural zinc. In order to achieve a no carrier added product with high specific activity, the backing was coated with a gold layer. After 190 µAh of bombardment, 61Cu was produced with an activity of 33.3 mCi/ µAh and high radioisotopic purity.

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Posters (T1/S6) 160 Optimization studies on the receovery of carrier-free iodine radioisotopes from irradiated tellurium-di-oxide by thermodistillation technique for application in routine production of radioiodine for biomedical applications S. Pal1, S. Chattopadhyay2, M.K. Das2, M. Surdersanan3 1Bhabha Atomic Research Centre (BARC), Analytical Chemistry Division, VECC, Kolkata, India 2Board of Radiation & Isotope Technology (BRIT), Radiopharmaceuticals, Kolkata, India 3Bhabha Atomic Research Centre (BARC), Analytical Chemistry Division, Mumbai, India Therapeutic and diagnostic applications of different isotopes of radioiodine, produced by accelerator as well as nuclear reactor irradiation, are well known. The current work describes the optimization studies carried out at our laboratory at Variable Energy Cyclotron Center, Kolkata, India to standardize a method for the recovery of radioiodine in carrier-free form from irradiated tellurium (IV) dioxide (TeO2) matrix utilizing dry thermodistillation technique. For standardization work, 131I radioisotope, produced by thermal neutron irradiation of natural TeO2 in Dhruva research reactor (neutron flux: 1014 n.cm-2.s-1) at Bhabha Atomic Research Centre (BARC), Mumbai, India, was used. The distillation of radioiodine (131I) from reactor irradiated TeO2 was carried out in a tubular quartz furnace at 750°C (slightly higher than the m.p. of TeO2, i.e. 733°C) and a distillation time of 15 min was observed to be ideal for volatilization of radioiodine under a stream of oxygen. The overall distillation yield of 131I was found to be higher than 80 % and reproducible. Compared to the recovery of 131I from irradiated Te metal powder, the yield from oxide of Te was found to be nearly three times. Different long lived radioisotopes of Te (i.e. 121Te, 123Te and 129Te), produced by (n, γ) nuclear reactions, were used to monitor the level of co-distilled Te in the separated 131I distillate and the inactive Te content was found to be in the range of 1-2 µg. Thermogravimetric Analysis (TGA) and Differential Thermal Analysis (DTA) of TeO2 and a mixture of TeO2 with 6% Al2O3, performed up to 750°C, provided data on the thermal effects on these matrices which are important information to set the distillation temperature for obtaining better yield of radioiodine distillate with minimum loss of irradiated TeO2 as well as making improved targets for the production of important cyclotron produced radioiodines. The thermal distillation method of isolation of radioiodines from irradiated TeO2 matrix is simple and ecologically safe technique for routine production of important iodine based radiopharmaceuticals using both cyclotron and nuclear reactor. This separation procedure generates minimum radioactive waste and recovers expensive enriched Te target material for reusing during production of 123I / 124I in cyclotron. 161 Separation of carrier-free radioactive multitracers from heavy-ion irradiated germanium target: applicability for the standardization of separation technique for routine production of PET radioisotopes S. Pal1, S. Chattopadhyay2, M.K. Das2, M. Sudersanan3 1Bhabha Atomic Research Centre (BARC), Analytical Chemistry Division, VECC, Kolkata, India 2Board of Radiation & Isotope Technology (BRIT), Radio-pharmaceuticals, Kolkata, India 3Bhabha Atomic Research Centre, (BARC), Analytical Chemistry Division, Mumbai, India In recent years, Positron Emission Tomography (PET) has been gaining considerable significance in diagonistic nuclear medicine, metabolic studies and drug evaluation. Among various positron emitting radionuclides, radioisotopes of yttrium (86Y), strontium (83Sr) and rubidium (82Rb) are potentially useful β+-emitters that find important applications in PET. In the present work, heavy-ion induced nuclear reactions have been applied for the simultaneous production of radioisotopes of yttrium (86Y, 87mY, 87Y, 88Y), strontium (83Sr, 85Sr) and rubidium (82mRb, 83Rb, 86Rb) from natural germanium oxide (GeO2) target by

irradiation with medium energy 16O6+ heavy-ion beam (~ 7 MeV/amu) at Variable Energy Cyclotron (VEC), Kolkata, India. The simultaneous production of radiotracers of Y, Sr and Rb from natural Ge-target through various nuclear reaction channels, like (16O, xn) or (16O, xpyn), were confirmed by γ-spectroscopy. Suitable radiochemical separation schemes were designed for the isolation of these individual radioisotopes in carrier-free form from the bulk irradiated Ge-matrix. For PET applications, 86Y-radionuclide is generally produced via 86Sr(p, n)86Y nuclear reaction using enriched 86SrCO3. The carrier-free radiotracers of Y and Sr, obtained by heavy-ion irradiation of Ge-matrix, were used in the present study to standardize a radiochemical separation technique for the isolation of Y radioisotope from Sr-matrix that could be applied for the routine production of 86Y- radioisotope for PET application by proton activation of enriched 86Sr-target as well as for the recovery of enriched target material after irradiation. The application of heavy-ion produced Y and Sr radiotracers were found to be useful to assess the efficiency of the separation scheme that yielded a satisfactory result with the separation of about 88% yttrium and recovery of 85% of strontium carbonate. Posters (T1/S7) 162 On the isotopic structure of semiconducting materials for spintronics and a solid-state quantum computer A. Tikhomirov Russian Research Center "Kurchatov Institute", Institute of molecular physics, Moscow, Russia A new direction in physics of condensed media that has been intensively developed in the recent years studies the controllability of electronic and nuclear spin states in various practical applications. Today the theoretical designs of transistors and memory units based on spin effects have been already developed. One of the most promising areas in spintronics is the development of a quantum computer. The basic principle of constructing the quantum computer is to arrange an ensemble of atoms or ions so as to allow their quantum states to be recorded and affected. There exist different possibilities to realize this principle, including a semiconductor variant based on Kane's scheme. It implies the ordered arrangement of NMR-active atoms with the odd nuclear spin (phosphorus-31) in silicon containing only the even silicon-28 isotope. According to Kane's proposal, the silicon must be monoisotopic. Silicon-28 is for the most part naturally abundant. The presence of its neighbour, silicon-29, having the odd nuclear spin is an impediment in the structure of the silicon quantum computer. The contribution of separation technologies to overcoming this impediment consists in producing the desired isotopic material. As it is impossible to obtain an enriched product containing 100% of the desired isotope, the task is to minimize the presence of impeding isotopes. An increase in isotopic purity will naturally require the greater volume of separation work. The concept of the solid-state silicon-28-based quantum computer is not the only possible one. Alternatively, a spinless matrix material and atoms suitable to form a quantum ensemble should be chosen. Germanium free of the germanium-73 isotope could be used as the matrix material for the quantum computer. Germanium-70 is the most suitable isotope for this purpose, because it has a sufficient natural abundance and is not neighboured with germanium-73. The comparison study of the production of isotopically pure silicon and germanium (bearing in mind the absence of odd-spin isotopes: silicon-29 and germanium-73) has been carried out in this work. As a separation method, the centrifugal separation has been only considered, because it has been used in Russia for more than thirty years to produce stable isotopes including silicon and germanium isotopes.

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163 Oxygen and carbon isotopes composition measurements by tunable diode laser spectroscopy methods G. Grigoriev1, S. Nabiev1, S.L. Malyugin1, A.L. Ustinov1, A.I. Nadezhdinskiy2, Y. Ponurovskiy2, D.B. Stavrovskiy2 1Russian Research Center "Kurchatov Institute", Institute of Molecular Physics, Moscow, Russia 2A.M. Prokhorov General Physics Institute, RAS, Natural Sciences Center, Moscow, Russia This report suggests a prototypes of the devices intended for rapid analysis of the water isotope composition (H2

16O, H217O, H2

18O, HD16O, HD18O, D2

16O, D218O) and carbon isotopes ratio

measurements 13CO2/12CO2 from the absorption spectra in the near-infrared range. Spectra are registered by tunable diode lasers (DL). The operating principle of a DL-based devices is as follows. DL lasing with the distributed feed-back in the range of 1.39 µm is effected with trapezoidal pulses of 0.5-2 ms duration and 10-30 kHz repetition rate. Frequency tuning in the DL radiation mode (~1.5 cm-1) occurs due to warming up of the lasing region of a crystal during the travel time of a pump current pulse. The lasing frequency domain (7183.2-7185.0 cm-1) has been chosen to ensure simultaneous detection of five isotopes. Vapors of water samples with various isotope contents are inlet, under pressure from 3 to 10 Torr, in parallel into two cells with optical paths of 100 and 10 cm, accordingly. A 100-cm cell is intended for measuring the water isotope composition at low isotope content (from 0.037 to 0.5 %). The other cell is used for measuring high isotope contents (0.5-99.9%). Absorption spectra of water isotopes are detected and then processed with a DAC/ADC board using the LabVIEW graphical package drivers. The time of a single measurement interval of isotopic ratio factors is ~0.5 s. On 100-times accumulation and averaging of these magnitudes, the final inaccuracy of definition of water isotope composition factors makes 0.1 % of the measured parameter. Similar DL (but with other wavelength λ=1.6 µm) with distributed feed-back and fiber radiation outlet and multipass optical system with the total optical path of 44 m were used for 13CO2/12CO2 measurements. Absorption lines R4 12CO2 and P12 13CO2 located in the frequency range of 6232.7-6232.5 cm-1 were monitored. Then an absorption ratio of these lines was measured, this ratio being proportional to magnitude of δ (‰) defining a change of the 13CO2/12CO2 isotopic ratio. The time of a single measurement of δ is maximum 0.2 s. After accumulation and averaging of the single measurements results the relative error of δ was within 0.7 ‰ that is quite acceptable for breath test diagnostics. 164 Enrichment of Ni-58 by electromagnetic isotope separator M. Mohati, A.J. Novinrooz, H. Bakhtiari, Z. Asadollahi, H. Sadri, M. Ghasemi, H. Seyedi Atomic Energy Organization of Iran, Nuc. Res. Center for Agriculture & Medicine, Material & Ion Beams Applications, Karaj, Tehran, Iran Enrichment of nickel isotope (Ni-58) has been carried out by the 180 degrees electromagnetic isotope separator for first time in Iran. Ni-58 is used as a target to produce Co-57 by cyclotron machine. Anhydrous nickel chloride as charge material was used in a graphite crucible of calutron ion source. It was evaporated at 300 ~ 500 degrees centigrade and ionized by bombarding 300eV electron beams emitted from a hot cathode. Ions were extracted with 30keV energy in vacuum tank at 1x10e-3 Pa pressure under 1280 gauss magnetic field and reached to collector after traversing 180 degrees circular path. Copper pockets and graphite front plate of collector was designed and fabricated for five isotopes of nickel. Profile of beams in collector position was determined by a faraday cup array. Some chemical procedures such as electro-deposition, ion exchange and organometallic precipitation was performed for recovery and purification of collected isotopes. High pure nickel oxide as final products for Ni-58 with more than 99.5% isotope abundance has been confirmed by ICP-AE, XRD and mass spectrometer.

165 Enrichment of stable isotopes utilizing the plasma separation processs F. Tarallo, N. Stevenson, T. Bigelow Theragenics Corporation, Oak Ridge, TN, U.S.A. The Plasma Separation Process (PSP) has been reassembled and is operational in Theragenics Corporation's® Oak Ridge, TN, facility. The PSP was formerly used in the U.S. Department of Energy's (DOE) Advanced Isotope Separation program, and is being leased by Theragenics™ from the DOE. The PSP utilizes mass discrimination to separate stable metal isotopes and is believed to be the only such process of its scale currently in operation. Key portions of this process include a microwave system that provides electron cyclotron resonance heating to form the plasma, an ion cyclotron resonance frequency system used to excite the desired isotope mass, and a 44-ton superconducting magnet capable of generating a magnetic field of up to 2 tesla. The PSP is designed to separate relatively large quantities of stable metal isotopes at moderate to high enrichment levels, and is capable of separating isotopes of most metallic elements. System and operational improvements are being considered that could increase throughput and enrichment capabilities. Theragenics™ also has laboratory facilities at the PSP site capable of harvesting the isotopes from the process and performing mass spectrometry analysis. Theragenics™ has successfully operated the PSP, most recently for the separation of 102Pd. Enriched 102Pd can be used as a precursor for the production of 103Pd, the radioisotope used in TheraSeed®, which is Theragenics'™ medical device used primarily to treat early-stage prostate cancer. Theragenics™ has also utilized the PSP to separate certain isotopes of gadolinium, erbium and dysprosium, for use as burnable poisons, as well as for certain nickel, copper and molybdenum isotopes. Other industrial, medical and research opportunities are also being considered. The opportunities for beneficial uses of isotopes is enhanced with the capabilities of the PSP, possibly including applications that may have previously been overlooked or rejected as being impractical. In addition to Theragenics'™ operational experience to date, potential PSP applications and capabilities will be discussed. Posters (T1/S8) 166 The disposal of radioactive medical waste at the waste repository in South Africa W. Meyer NECSA, Radiochemistry, Pretoria, Gauteng, South Africa Vaalputs is a national, near surface, radioactive waste management facility that serves South Africa's needs for disposing off low and intermediate level short lived, radioactive waste generated by Koeberg nuclear power station. Another shale site "Thabana", acts as a temporary storage facility for containers containing trans-uranic waste, radioactive waste from hospitals, industrial and agricultural waste, as well as radioactive waste from other research institutions such as universities. 14C, 129I and 99Tc are the most important radionuclides in the global scale long term radiological assessment of a waste repository. These nuclides have long half-lives, 5 730 years, 1.6 x 107 and 2 x 105 years, respectively, and readily migrate through ecological environments, achieving widespread distribution. 14C is also an important radionuclide for regional radiological assessment because it gives a significant fraction of the effective dose to general public through atmosphere-agricultural food-ingestion path. For the determination of the feasibility of disposal of medical radioactive contaminated wastes at Vaalputs, it was necessary to determine the distribution coefficients of these medical radionuclides under different redox conditions at this geological waste repository as the backfill used contains high Chloride and Sulphate concentrations. The results obtained on the site-specific Vaalputs soil correspond with the trends observed in the literature and indicate that different soil conditions, concentration and redox conditions have a

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relatively minimal effect on the Kd values. The very low distribution coefficient Kd values observed for 131I, 99mTc and 14C can be attributed to a repulsion and ion exclusion mechanism. The results indicated that these medical species will migrate through the Vaalputs environment toward the groundwater and therefore disposal of medical waste at Vaalputs can only be accommodated in the presence of engineered barriers. 167 Production of metal ruthenium from irradiated technetium K.V. Rotmanov1, L.S. Lebedeva1, V.M. Radchenko, V.A. Tarasov, E.G. Romanov1, Y.G. Toporov1, V.F. Peretroukhin2, A.A. Kozar2 1Federal State Unitary Enterprise State Scientific Centre - Research Institute of Atomic Reactors, Russia 2Institute for Physical Chemistry RAS, Moscow, Russia A number of experimental irradiations have been carried out during last two years under the active program of research. A set of technetium targets as metal discs of 6 mm in diameter and 0.3 mm thickness was irradiated in the neutron trap of the SM high flux reactor at RIAR. The targets were unloaded from the reactor in three batches after each of them has achieved desirable burn-out value. The irradiated samples have been found to be technetium alloys containing 19, 45, and 70% of ruthenium. Results of chemical reprocessing irradiated targets and obtaining artificial ruthenium metal are presented in the report. Targets were dissolved in the potassium hydroxide solutions containing potassium periodate KIO4 followed by precipitation of ruthenium (IV) hydroxide adding of ethanol. To purify it from technetium impurity ruthenium was distilled as RuO4 into the ethanol solution, where it reduced and precipitated as ruthenium (IV) hydroxide. To obtain metal ruthenium Ru(IV) hydroxide precipitate was converted to dioxide RuO2 and reduced to the metal state in hydrogen atmosphere at 400 C. The isotopic composition of prepared artificial metal ruthenium depending on technetium burnout was found to be as follows: Technetium burn-out, %

100Ru content, % 101Ru Content, %

19 45 70

98.93 97.94 97.42

0.54 1.35 1.79

Content of heavy ruthenium isotope, like 102Ru and 104Ru, did not exceed 0.8%. So, ruthenium metal prepared seems to be practically mono-isotope. Thus it differs from natural ruthenium having seven stable isotopes. 168 Successful experiments and controlled decontamination of water mixture of different long-lived active isotopes by transmutation in biological cells V.I. Vysotskii1, A. Odintsov2, V.N. Pavlovich3, A.B. Tashirev4, A.A. Kornilova5 1Kiev Shevchenko Univ., Kiev, Ukraine 2Institute of problems of NPP safety, Kiev, Ukraine 3Kiev Institute of Nuclear Research, Kiev, Ukraine 4Kiev Institute of Microbiology, Kiev, Ukraine 5Moscow State University, Moscow, Russia In the work the process of direct controlled decontamination of highly active water mixture of selected different long-lived active isotopes by action of growing microbiological systems has been studied. The process was connected with transmutation of long-lived active nuclei to non-radioactive isotopes during growth and metabolism of special microbiological MCT ("microbial catalyst-transmutator"). The MCT is the special granules that include: concentrated biomass of metabolically active microorganisms, sources of carbon and energy, phosphorus, nitrogen, etc., and gluing substances that keep all components in the form of granules stable in water solutions for a long period of time at any external conditions. The base of the MCT is microbe syntrophin associations of thousands different microorganism kinds that are in the state of complete symbiosis. These microorganisms appertain to different

physiological groups that represent practically the whole variety of the microbe metabolism and relevantly all kinds of microbe accumulation mechanisms. The state of complete symbiosis of the syntrophin associations results on the possibility of maximal adaptation of the microorganisms' association to any external conditions change. The typical reaction of the association for such aggressive effects demands some time for internal adaptation. This time is necessary for mytagene change of about 10 generations that corresponds to several days. During this time occurs a purposeful synergy process of stimulation of the mutant formation of such microorganisms that are maximally adapted to the changed aggressive conditions. The mechanism of nuclear transmutation in growing biological system is described in [1]. The research has been carried out on the basis of the same distilled water that contained four long-lived reactor isotopes: Eu154 (initial activity about 700 bq), Eu155 (≈300 bq), Cs137 (≈2.104 bq), Am241 (≈1500 bq). In our experiments 8 identical closed glass flasks with 10 ml of the same active water in each were used. The "microbial catalyst-transmutator" was placed in 7 glass flasks. In six different flasks different pure K, Ca, Mg, Na, Fe and P salts as single admixture were added to the active water. These chemical elements are vitally necessary for any cultures. Each of these replacements completely blocks the channel of transmutation with the use of all biochemical analogs of the concrete chemical element [1]. The results obtained confirmed the importance of such replacements. Two additional flasks were used for control experiments: one flask contained the active water and MCT (but without salts) and in another one was only active water (without salts and MCT). The cultures were grown at the temperature 25° C. Activity of all closed flasks has been measured every 7 days by amplitude Ge detector during 6 months. The results of controlled influence on gamma-radioactivity of different isotopes in different biochemical compositions are reported. We have observed speeded up decay of Cs137 isotope in all experiments with MCT and with the presence of different additional salts. The most speeded up decay with τ* ≈310 days (accelerated by 12 times) was observed at the presence of Ca salt. [1]. Vysotskii V.I., Kornilova A.A. Nuclear fusion and transmutation of isotopes in biological systems, Moscow, "MIR" Publishing House, 2003, 302 p. 169 Design-experimental validation of minor-actinides transmu-tation in the BOR-60 reactor A.A. Mayorshin, V.A. Kisly, O.V. Shishalov, V.N. Efimov, I.Y. Zhemkov, A.A. Teykovtsev, V.V. Dvoretsky, F.N. Krukov, A.E. Novoselov RIAR, Dimitrovgrad-10, Russian Federat In accordance with the closed fuel cycle concept the SSC RF RIAR carries out activities on design-experimental validation of long-lived MA (Np, Am, Cm) transmutation by irradiating in fast reactors. Effectiveness of Np and Am transmutation has been calculated both for the BOR-60 core and blankets depending on energy spectrum of neutrons. Experimental batch of granulated UNpO2 - fuel with Np content, less than 5%, has was produced by using pyroelectrochemical reprocessing in the molten salts. Main characteristics of this batch meet the requirements for vibropac fuel pins fabrication. This fuel was used for fabricating two experimental fuel pins. The fuel pins were incorporated in dismountable fuel assembly of the BOR-60 reactor and irradiated under the parameters similar to those of standard fuel pins. Two fuel pins with the burnups of 13.7 % and 19.5 % h.a. have been investigated using nondestructive and destructive techniques. From results of the investigations both fuel pins are found to be leak-tight. Taking into consideration irradiation conditions, the paper presents results of investigations of Np and Am burning out effectiveness in the neutron spectrum of the BOR-60 reactor and PIE results for UNpO2 fuel pins. Besides, kinetic laws of neptunium and americium transmutation in the BOR-60 core are shown.

5ICI April 25 – 29, 2005 51

Results of in-pile tests and PIE indicate, that there are no significant differences in the efficiency of UNpO2 fuel pins as against fuel pins containing UO2 or UPuO2 fuels. Posters (T1/S9) 170 The use of isotopic neutron sources for some radionuclides production in nuclear medicine and other domains of science L. Daraban, L. Daraban, O. Cozar, R. Adam-Rebeles University Babes-Bolyai, Faculty of Physics, Cluj-Napoca, Romania The isotopic neutron sources of 241Am- 9Be and 239Pu- 9Be type was used for some radionuclides production such as: 116mIn, 198Au, 62,64Cu,56 Mn, 122,124Sb, 152mEu, 187W, 75mGe, 111mCd, 87mSr by irradiation with thermal and fast neutrons. We also recorded their gamma spectra using a Ge(Li) detector and we drawn their disintegration curves in order to determine their half-lives. We identified also the disintegration schemes and we calculated the specific activity of these radioisotopes. In order to estimate the performance of these isotopic neutron sources, we will provide some proposals regarding their application in laboratories. 171 Gamma-ray design with Am-Be neutron source M. Jalali Esfahan Nuclear Fuel Research & Production Center - Atomic Energy Organization of Iran, Nuclear Engineering Department, Esfahan, Iran Thermal neutron intraction with nuclides elements, produces prompt gamma ray up to 11 MeV. Ni element in this reaction produces gamma ray in the range 7-9 MeV with suitable yield. Shielding and reflector of Am-Be with Ni cylinder above neutron source have been simulated with MCNP-4C code. The best thickness of Ni and paraphine upper reflector have been calculated as 27.6 mm and 70 mm respectively. This calculations have been compared with the same experiments in TRIUMF center. 172 Experimental methods for measurement β-pure radionuclides P. Van den Winkel1, L. Daraban2 1Eenheid Cyclotron, Vrije Universiteit Brussel, Belgium 2Faculty of Physics, University Babes-Bolyai, Cluj-Napoca, Romania The plastic scintillator b-spectroscopy was applied to the waste measurements by using a large area of 45x48.5x4 cm plastic scintillator. One of most important problem is the calibration of the multichannel analyzers regarding to beta ray energy units. It is also described a very simple method for calibration of plastic scintillators by using the Compton electron distribution regarding to the end-point method. In order to proceed the deconvolution, it was prepared a program for processing these spectra by Fermi-Kurie plots and a special representation of Fermi function. Thet method of calibration is in good agreement with the results obtained by other techniques and provides the maximum energy of β-radiation. Our method was adapted for measurements in regions of interest with different β-energies from large radioactive waste samples. 173 Excitation functions of longer lived products in deuteron induced nuclear reactions on platinum up to 40 MeV F. Ditrói1, J.-F. Tárkányi1, J. Csikai1, M.S. Uddin2, M. Hagiwara2, M. Baba2, Y.N. Shubin3, S.F. Kovalev3 1Institute of Nuclear Research of the Hungarian Academy of Sciences, Debrecen, Hungary 2Cyclotron and Radioisotope Center, Tohoku University, Sendai, Japan 3Institute of Physics and Power Engineering, Obninsk, Russian Federation

In the frame of a systematic study of excitation functions of light charged particle induced nuclear reactions on metal targets in the medium energy range production cross-sections for deuteron induced nuclear reactions were investigated. In our previous work we investigated these reactions up to 21 MeV. In the present work the energy range was extended up to 40 MeV [1]. No other experimental activation cross-section data are known in the literature. The main reaction products in this energy range mostly belong to radioisotopes of gold and platinum. Platinum is frequently used in different nuclear technology as target backing, collimator for low background neutrons, part of different sensors, catalyst, etc, Radionuclides of gold are used for therapeutic purposes (198Au,199Au). The radionuclides of platinum (191Pt, 193mPt,195mPt) are also used for therapy and to follow biodistribution of platinum compounds. Medical applications require microscopic data on monoisotopes, but according to the experience the elemental data are very important to estimate the production yields and impurity levels. Our investigations were performed in the frame of systematical study of production cross-sections on metals for developments in accelerator related technologies (activation analysis, thin layer activation technique, dose calculations, waste disposal, etc). A physically accurate activation method on stacks of natural platinum target foils was used. The target stacks were irradiated at the cyclotron of the Tohoku University, Sendai. Precise determination of the effective particle energy and possible corrections to the beam intensity was obtained by re-measurement of the well known 27Al(d,x)22,24Na and natCu(d,x)65Zn excitation functions over the whole energy range and simultaneously fitting to the reference values. As a result excitation functions were determined from the respective threshold up to 40 MeV for the natPt(d,x)191,192,193,194195196m,196,198,199Au, natPt(d,x)191,195m,197Pt and natPt(d,x)188,189,192Ir reactions. The new cross section data are in good agreement with our earlier result at the low energy overlapping energy range. The experimental cross sections were compared with the result of model calculation by means of computer-code ALICE-IPPE. The physical yields and thin layer activation curves for the measured activation products were calculated from the experimentally measured excitation functions for pure Pt metal target. The possible alternative uses in medically relevant radionuclide production as well as applications in thin layer activation and dosimetry will be discussed. [1] F. Tárkányi et al. Nucl. Instr. Meth. B 226 (2004) 490 174 Compilation and evaluation of nuclear reaction cross sections for production of therapeutic radioisotopes F. Tárkányi1, E. Betak2, R. Capote3, B.V.,Carlson4, H.-D. Choi5, E. Menapace6, F.M. Nortier7, R. Paviotti de Corcueara3, S.M. Qaim8, B. Scholten8, Y.N. Shubin9, J.-C. Sublet10 1Institute of Nuclear Research of the Hungarian Academy of Sciences, Debrecen, Hungary 2Institute of Physics, Slovak Academy of Science, Bratislava, Slovakai 3Nuclear Data Section, IAEA, Vienna, Austria 4Instituto Technológico de Aeronáutica Praca Mal. Eduardo Gomes, Sao Jose dos Campos SP, Brasil 5Department of Nuclear Engineering, Seoul National University, Seoul, Korea 6ENEA-Division of Advanced Physics Technologies, Bologna, Italy 7Los Alamos laboratory, C-INC: Isotopes and Nuclear Chemistry Group, Los Alamos, USA 8Institut für Nuklearchemie, Forschungszentrum Juelich GmbH, Juelich, Germany 9Theory Division, Institute of Physics and Power Engineering, Obninsk, Russia 10CEA, Cadarache, France A cross section database for the production of therapeutic radionuclides is under development in the frame of an IAEA-Coordinated Research Project (CRP). The project can be considered as a continuation of the previous CRP which concentrated on the

52 April 25 – 29, 2005 5ICI

production of medically related diagnostic radioisotopes and charged particle beam monitor reactions [1]. Out of a significant number of radionuclides in use or being proposed for therapeutic applications, the project focuses on the production of the most important established and emerging radioisotopes (and the associated critical impurities). The list of reactions includes nearly fifty important neutron and charged particle induced reactions. The program of work consists of new measurements, compilation, critical selection and fitting of the available data, nuclear model calculations, and validation of the recommended data. The database will be available on web and will be published as an IAEA TECDOC. The new experimental data will be published separately in dedicated journals. The status of the program will be reviewed. [1] Charged particle cross-section database for medical radioisotope production: diagnostic radioisotopes and monitor reactions. Vienna, IAEA. IAEA-TECDOC- 1211 (2001) (http://www.nds.or.at/medical) 175 Cf-252 half-life measurement M. Jalali Esfahan Nuclear Fuel Research & Production Center - Atomic Energy Organization of Iran, Nuclear Engineering Department, Esfahan, Iran The method used for half-life measurement of Cf-252 is based on the production of prompt gamma ray from the source neutron reaction with its paraphin standard shield. By analysis of the prompt gamma ray spectrum data gathered in the energy range 3-8 MeV with NaI detector, the half-life of Cf-252 is determined to be 2.77 years. 176 Activation cross sections of deuteron induced nuclear reactions on iridium F. Tárkányi1, B. Király1, F. Ditrói1, S. Takács1, J. Csikai1, A. Hermanne2, M.S. Uddin3, M. Hagiwara3, M. Baba3, Yu.N. Shubin4, S.F. Kovalev4 1Institute of Nuclear Research of the Hungarian Academy of Sciences, Debrecen, Hungary 2Vrije Universiteit Brussel, Brussels, Belgium 3Tohoku University, Cyclotron and Radioisotope Center, Sendai, Japan 4Institute of Physics and Power Engineering, Obninsk, Russia Excitation functions of deuteron induced nuclear reactions on iridium were measured for practical applications up to 40 MeV. No earlier experimental data have been found in the literature for activation cross sections of low energy deuteron induced reactions on Ir. This work was performed in the frame of a systematic study of excitation functions of light charged particle induced nuclear reactions on metal targets in the medium energy range. In our previous work the results of proton induced reactions on iridium up to 70 MeV were reported [1]. The cross-sections on iridium were measured by using a standard stacked foil irradiation method. The irradiations were carried out on low intensity external beams of the cyclotrons at the Tohoku University, Sendai and at the Vrije Universiteit Brussel, Brussels. Al, Ti and Cu foils were inserted into the stack as energy degraders and as monitors of the beam parameters. The γ-spectra of the irradiated iridium and monitor foils were measured non-destructively on a high purity Ge detector. The counting was started 2 hours after EOB (end of bombardment) and continued for several weeks. It allows following the decay of isomers and parent radionuclides and decomposition of gamma-lines originating from different isotopes. The beam intensity and the energy degradation along the stack were controlled via the natAl(d,x)22,24Na, natTi(d,x)48V natCu(d,x)65Zn monitor reactions. So called elemental cross-sections were calculated by supposing the target to be monoisotopic. Direct and cumulative cross-sections were deduced from the parameters of the bombarding beam and of the target taking into account the decay data of the radionuclides involved. As a result we present excitation functions for the natIr(d,xn)188,189,191Pt and natIr(d,x)188,189,190,192,194Ir nuclear reactions

up to 40 MeV deuteron energy. The measured experimental data were compared with theoretical calculations based on the model code ALICE-IPPE. The physical yields and thin layer activation curves for the measured activation products were calculated from the experimentally measured excitation functions for pure Ir metal target. Application of the measured experimental data in different fields (industry, medicine) will be discussed. [1] F. Tárkányi et al., ND2004 Conference, Santa Fe, USA, 2004, Abstracts, p.137 177 Construction of Korean male phantom and organ absorbed dose measurement J. Kim1, H. Choi1, B.I. Lee1, Y.K. Lim1, C.S. Kim1, C.S. Lee2, J.K. Lee2 1Radiation Health Research Institute, Health Physics Lab, Seoul, Korea 2Hanyang University, Nuclear Engineering, Seoul, Korea The first Korean physical phantom for radiation protection purposes was constructed using computed tomography images of a healthy volunteer, whose body dimension was closed to that of average Korean male. The volunteer's whole body CT scan images were obtained from PET/CT facility in Radiation Health Research Intitute (RHRI). The CT data in DICOM format of whole body except arms and legs was converted into STL format in order to be ported to Rapid Prototyping (RP) machine for manufacturing the phantom. The resulting physical phantom was composed of three tissue equivalent materials: epoxy resin, urethane foam, and poly urethane representing bone, lungs and soft tissues, respectively. The density of the materials was close to those recommended by International Commission on Radiation Units and measurements (ICRU). The resulting phantom was sliced horizontally by the thickness of 2cm into 43 slices. Each slice had the holes for location of Thermo Luminescence Dosimeter (TLD) by 2 cm interval, which was calculated by Monte Carlo method. To verify the appropriateness of the physical phantom, organ doses of selected organs were measured for reference photon beam, and compared with those computed by Monte Carlo method with the voxel model constructed from the same CT images. Abosrbed doses converted from TL relative response showed good agreement within 7% with those calculated.

5ICI 53 Poster Session II: Labelled Compounds, Synthesis & Applications

Posters (T2/S1) 178 Optimized synthesis of thyroid hormones labelled with carbon-13 A. Hantson, M. De Meyer Faculté Polytechnique de Mons, Applied Chemistry and Biochemistry, Mons, Belgium Former thyroid clinical studies involving radioactive molecules (131I or 125I) exhibit potential hazard for human health and induce ethical problems. The use of stable isotope labelled molecules allows safe in vivo tracing and precise metabolism investigations. Our main objectives are the production of labelled thyroid hormones (T4-13C, thyroxine-13C) and the development of analytical protocols for their quantification in biological fluids. The synthesis scheme of T4-13Cx (3, 3',5,5'-tétraiodothyronine) and T3-13Cx (3, 3',5-triiodo-thyro-nine), with the best chemical and optical purities, is achieved under homogeneous and supported conditions (solid phase synthesis) with diaryliodonium salt, copper catalyst, tritethylamine in methanol. The precursor is L-tyrosine which is commercially available and can be bioproduced with 13C labelled phenol and pyruvate as starting materials. After optimization of homogeneous phase synthesis, we are able to produce the T4-13Cx with an overall yield of 50 % and T3-13Cx with 30 % yield. Solid phase protocol does not lead to yield improvement. Due to the high cost of the labelled precursors, the synthesis is improved to limit the losses of starting labelled materials. Intermediates quality is confirmed by HPLC and GC-MS analysis. For the in vivo study, the crude labelled thyroxine is purified by recrystallization and liquid chromatography. The labelled thyroid hormones obtained have a high optical purity: 97 ± 2 % L-T4-13Cx. This synthesis scheme allows the production of thyroid hormone products characterized by various isotopic enrichments in carbon 13, but also in nitrogen 15 and oxygen 18. These optically active biomolecules can be used as in vivo tracers for new thyroid metabolic studies and as internal standards for analytical reference methods. New analytical techniques such as isotopic dilution coupled with GC-MS and HPLC-MS/MS are appropriate tools for their detection and quantification in biological fluids and give the opportunities to record data on metabolic degradation pattern of the labelled molecules (T3, T4). 179 Preparation of new 1-(4-Sulfonamidophenyl)-5-aryl-1,2,3-Triazole(5-14C) derivatives as COX-2 selective inhibitors F. Johari Daha, H. Matloubi, N. Saemian, G. Shirvani Nuclear Research Center / AEOI, Chemical Division, Tehran, Iran Two isoforms of cyclooxygenase (COX) enzyme have been identified1. Non-selective inhibition of these enzymes with non-steroidal anti-inflammatory drugs2 (NSAIDs) is often accompanied by GI and renal side effects. Selective inhibition of COX-2 would constitute a novel approach to the treatment of inflammation with diminish side effects3. Based on the structures Activity Relationship for selective COX-2 inhibitors the following compounds were designed and labeled with carbon-14 in order to elucidate the mechanism of action and metabolism studies4. The desired products, were synthesized according to the synthetic pathway shown in following scheme5,6,7,8.

Ba14CO3 K14CN Cu14CN X I

X 14CNX 14CO

H

NH2S

14CN

XS

H N

NN

H14C

S

a b

c

d

e

O

O

N

Bz

Bz

N

O

O Bz

Bz

X

NO

O

Bz

Bz

N

NN

14C

SX

NO

O

Bz

Bz

N

NN

14C

SX

NH2O

O

f

g

h

X=H, -CH3, -OCH3

a) K, KN3. b) CuSO4, Na2S2O5. c) DMF. d) Raney-Ni, HCO2H. e) EtOH/THF. f) CH2N2, Dioxane. g) KMnO4, n-Bu4N+Cl-, Benzene, H2O. h) H2O4(Conc.) 1Kadaba, P.K., J. Med. Chem. 1988: 31, 196 2Li, J.J., Nortone, M.B., et al. J. Med. Chem. 1996: 39, 1846 3Talley, J.J., et al. J. Med. Chem. 2000: 43, 775 4Sunay, U.B., et al. J. Labelled Compd.Radiopharm. 1992: 31, 1041 5Matloubi, H., Saemian, N. et al. Appl. Radiat. Isot. 2002: 57, 501 6Matloubi, H. Shirvani, G. et al. J. Labelled Compd. Radiopharm. 2002: 45, 347 7Matloubi, H., Saemian, N., Shirvani, G., Johari, F., Appl. Radiat. Isot. 2004: 60: 665 8Matloubi, H., Saemian, N., Shirvani, G., Johari, F., J. Labelled Compd.Radiopharm. 2004: 47, 31. 180 Synthesis of N-(2,3-dihydro-1-[14C]methyl-2-oxo-5-phenyl-1H-1,4-benzodiazepin-3-yl)-benzamide and N-(2,3-dihydro-1-[14C] methyl-2-oco-5-phenyl-1H-1,4-benzodiazepin-3-yl)-N-[14C] methyl-benzamide as novel carbon-14 labelled G. Shirvani, H. Matloubi, N. Saemian Nuclear Research Center / AEOI, Chemical Division, Tehran, Iran Dealkylayion and 3-hydroxylation are the most important metabolic routes for several 1,4-benzodiazepine derivatives. Isotopic substitution at the site of metabolic transformation is one of the best methods for elucidating the mechanism of the metabolic process and several carbon 14 labelled benzo diazepine derivatives have been synthesized and there metabolic fates studied in human and animal models1. Since the isolation of the non-peptidal cholecystokinin (CCK) antagonist Asperlicin, the 1,4-benzodiazepin ring system has served as a useful tool for delineating the pharmacologic action of CCK. In order to study the rate of 1-dealkylation of benzodiazepine CCK antagonist and its influence on the pharmacologic profile of this compounds it became necessary to synthesis a CCK antagonist derivate labeled with carbon-14 at the N-1 position. Furthermore in order to determine the rate of chain N-methyl dealkylation, synthesis of a ligand, N-methylated both in N-1 and the amide chain appeared of interest. The carbon-14 labelling step in synthesis of 2 and 3 consist of methylation of 1 [14C] methyl iodide, prepared by the known method2. From barium [14C] carbonate via [14C]methanol. The benzodiazepine CCK antagonist 1 was prepared through a benzotriazole-assisted synthetic route from benzamide and 2-aminobenzophenone. By utilization of molar equivalent of 1 and [14C]methyl iodide and a short reaction time, the mono methylated product 2 in which N-1 of the dibenzodiazepine ring is methylated, is obtained. Using [14C]methyl iodide in excess and extending the reaction time yields the dimethyl derivative. Biological studies of these compounds are currently under investigation3,4.

54 April 25 – 29, 2005 5ICI

N

HN

OHN

O14CH3I / NaH / DMF

N

NO

NO

R1

R2

1 Reaction time: 5 min.2 R1=14CH3 , R2=H 45min. 3 R1=R2 = 14CH3 1Maksay G, Tegyey Z, Otvos LJ Chem. Soc. Perkin Trans. 1988; 11:57 2Cox JD, Turner HS, J Chem Soc 1985; 3167 3Khalaj A, Pirali M, Matloubi H, Dowlatabadi R, Monatsh Chem 2001; 132: 747 4Matloubi H, Shirvani G, et al. J Label Comp Radiopharm 2002 ; 45 : 374 181 Synthesis of L-[C-13]amino acid M. Kajiwara1, K. Takatori, M. Lee, A. Hayashi 1Meiji Pharmaceutical University, Medicinal Chemistry, Tokyo (1). An Asymmetric Synthesis of L-[3-13C]Alanine, L-[3-13C]Phenylalanine, L-[3-13C]Tyrosine4, L- [2-13C]Aspartic acid, L-[ 4-13C]Lysine, and L-[ 3-13C]Tryptophan Stable isotope-labelled amino acids are useful for the diagnosis of disease, the study of the biosynthesis of natural products and other biological studies. We described asymmetric syntheses of L-[3-13C]alanine L-[3-13C]phenylalanine, L-[3-13C]tyrosine4 and L- [2-13C]aspartic acid, L-[4 -13C]lysine, and L-[3-13C]tryptophan from Dellaria's oxazinone6 or its 13C-labelled form as a chiral glycine equivalent. L-[3-13C]Alanine was synthesized from [13C]methyl iodide by using Dellaria's oxazinone, prepared from phenyl [2-13C]bromoacetate and (S)-2-phenylglycinol, as a chiral glycine equivalent. Alkylation of the oxazinone with [13C]methyl iodide was achieved with high diastereoselectivity. Hydrolysis and removal of the chiral auxiliary of the alkylated oxazinone gave L-[3-13C]alanine. L-[3-13C]Phenylalanine and L-[3-13C]tyrosine were synthesized. [ 13C]Benzyl bromides were prepared from [13C]carbon monoxide via the palladium-catalyzed carboalkoxylation of arylhalides. The asymmetric carbon corresponding to 2-position in phenylala-nine was introduced by the diastereoselective alkylation of Dellaria’s oxazinone with [ 13C]benzyl bromides. Finally, ethanolysis, deprotection, hydrogenolysis and acid hydrolysis of the resulting alkylated oxazinones gave L[3-13C]phenylalanine and L-[3-13C]tyrosine in high optical purity. L-[2-13C]Aspartic acid was synthesized by using Dellaria’s oxazinone labelled with 13C at the 3-position, prepared from phenyl [2-13C]bromoacetate and (S)-2-phenylglycinol. Phenyl [2-13C]bromoacetate was derived from sodium [2-13C]acetate. Alkylation of the [3-13C]oxazinone with ethyl bromoacetate was achieved with high diastereoselectivity. Finally, sequential deprotection and removal of the chiral auxiliary of the alklated [3-13C]oxazinone afforded L-[2-13C[aspartic acid. This method is also applicable to the synthesis of various amino acids with labelling at other positions. L-[4-13C]Lysine was synthesized from sodium [2-13C]acetate and Dellaria's oxazinone. Acknowledment: This study was supported in part by Grant-in-Aid for Scientific Research (No. 15590142) from the Ministry of Education, Science, Sports and Technology of Japan, and by The Science Research Promotion Fund from The Promotion and Mutual Aid Corporation for Private Schools of Japan. Posters (T2/S2) 182 Dihydrotestosterone labelled with tritium L. Matei1, C. Postolache1, V. Fugaru1, C. Podina2 1National Instiute for Physics and Nuclear Engineer, Radioisotope Production Centre, Bucharest, Romania 2University of Bucharest, Faculty of Chemistry, Bucharest, Romania Labelling of testosterone and dyhydrotestosterone with tritium was necessary for caring out of radiometric and molecular biology studies concerning androgen dependent diseases. Hormones labeled

with tritium, were obtained in two stages: 1) selective hydrogenation of 1-dehydro testosterone acetate in the presence of T2 gas, at low pressure, and 2) hydrolysis of the ester at basic pH. The raw labelled compounds were purified by preparative thin layer chromatography. Testosterone-1,2-T and dihydrotestoste-rone-1,2,4,5-T was obtained by chemical synthesis. Hydrogenation reaction was also analyzed by quantum chemical methods. Were determinated total binding energies of: reactants, transitional state and reaction products. Biologically active, dihydrotestosterone-1,2-T was obtained by biosynthesis using as substrate testosterone-1,2-T. Enzymatic activity of 5α reductase was studied using human skin and prostate tissue homogenates incubated 1h at 37°C with Testosterone-1,2-T. As cofactor we used NADPH. After reaction stopping, testosterone metabolites were extracted with a mixture of cyclohexane/ethyl acetate. Product separation was realized using Celite chromatographic columns. As mobile phase we used a mixture of isooctane/toluene. Labelled testosterone used as substrate in enzymatic reaction was purified by column chromatography using previous system. On collected fractions as result of chromatographic elution were determined enzymatic activities using a Packard Liquid Scintillation Counter. From radiochromatographic profiles were identified base peak of testosterone used as substrate, peaks of dihydrotestosterone, androstandione and also peaks of 3 α and 3β androstandiols with very low intensity. This study confirms the possibility of dihydrotestosterone and androstandione biosynthesis. Androstandiols can be also synthesised with low yields. 183 Synthesis of n-phenylsuccinimide labeled with hydrogen isotopes C. Postolache1, L. Matei1, V. Fugaru1, C. Deleanu2, N. Negoita1, V. Serban1 1National Institute for Physics and Nuclear Enginee, Radioisotope Production Centre, Bucharest, Romania 2Institute of Organic Chemistry, Organic Chemistry Centre, Bucharest, Romania N-phenylsuccinimide labelled with tritium was obtained by catalytic hydrogenation of N-phenylmaleinimide. The precursor was synthesized by condensation reaction between maleic anhydride in pyridine medium. The raw labelled compounds were purified by preparative thin layer chromatography, and product was characterized by determination of radioactive concentration, radiochemical purity, chemical concentration and specific activities. Tritium labelled compound was used in obtaining of radioluminescent sources. Deuterated compound was obtained by a similar methodology. Purification was realised by double crystallisation in alcohol. Product was analysed by IR spectrometry, RMN and used as GC MS internal standard. Experimental results were associated with quantum-chemical studies. In this study were analyzed: self-radiolysis stability of tritium labelled compound and spectral isotopic effects in deuterated compound. 184 The influence of depleted deuterium water on dna synthesis in rat bone marrow cells following citostatic chemotherapy V. Fugaru1, C. Postolache1, M. Lidia1, I. Encut2, M. Panait2 1Institute for Physics and Nuclear Engineering, Radioisotopes Production Center, Bucharest, Romania 2Institute of Oncology, Cancer Biology, Bucharest, Romania The usual concentration of deuterium in water is about 150 ppm D/D+H, over (16 mM) The mass difference between hydrogen and deuterium leads to difference in the physical and chemical behaviors between the two isotopes. Based upon the observation that concentration of deuterium in living organism is 40% less than usual water, we supposed that the cells are able to maintain these ratio, and the change in D/D+H ratio can trigger certain molecular mechanism. It is known that the decreasing the concentration of

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deuterium in the body of living animals can be achieved by a diet with depleted deuterium water (DDW). The aim of this study was to investigate the effects of diet with DDW 60 ppm on DNA synthesis in bone marrow cells of Wistar rats which where assessed by 3H-Thymidine incorporation. The Wistar rats were divided in two groups: the first group had a diet with normal distillated water and the second group a diet with DDW 60 ppm. Both groups of animals received a single chemotherapy treatment in therapeutic dose. 10 days after the end of citostatic chemotherapy 3H-Thymidine was injected intravenously (20 kBq/g of body weight). The animals were sacrificed and immediately after sacrifice, samples of femural bone marrow were obtained and processed to determine organically bound tritium (OBT) by liquid scintillation counting. Our results show a significant statistically increase of OBT- a measure of DNA synthesis- in the group of mice fed with DDW 60 ppm compared with control group. We suggest that the application of diet DDW 60 ppm may open new possibilities in cancer therapy as a protective therapy. Posters (T2/S3) 185 The production of I-125-progesterone tracer J.M. Wagener1, O. Perera2, M. Khadra2 1Necsa, Radiochemistry, Pretoria, South Africa 2IAEA, Animal Production and Health, Vienna, Austria The use of RIA technology for progesterone measurement in developing countries has been an ongoing project in a few African as well as Asian countries. The progesterone measurement is used for monitoring and improving of livestock production. The objective was to transfer a simple, robust and cheap RIA-method. The milk progesterone RIA system is based on a direct method using 125I-progesterone tracer and a solid phase separation method (antibody coated tubes), which is suitable for use in developing countries. This simplified RIA method can be performed in any laboratory with basic facilities for routine biochemistry or chemistry. The labs were equipped with the necessary instruments at a minimum cost of $5 000. The main reagents, antibody and tracer, are produced in bulk to cut cost of a usually expensive analysis method. Presently the antibody is supplied by IAEA Labs, while Necsa has been supplying the tracer (progesterone-11 -hemisuccinate-2(125I)-iodohistamine) since August 2003 to African counterparts. The advantages are the low cost, an easy, validated method to use bulk reagents for coating of tubes and performing the assay. 125I is widely used for preparation of iodinated tracers for sensitive immunoassays and receptor binding assays. Protein iodination can be done directly by using the soluble oxidizing agent chloramine-T. This is the most widely used method to radio-iodinate small amounts of protein to high specific radioactivities. It is a technically simple and rapid reaction. The steroid, progesterone-11 -hemisuccinate used for this application has no phenolic group present that can easily absorb iodide. It therefore needs to be activated with a -COOH group before labelling. This is a mixed acid, hydride reaction performed with isobutylchloroformate in dioxane at basic conditions by using N-methylmorpholine in dioxane. Histamine is used as the carrier molecule, which is iodinated with 125I using chloramine-T as the oxidizing agent. The resulting iodohistamine is directly coupled with activated progesterone. This conjugate 2-iodohistamine-11 -hemisuccinate progesterone is purified by ethyl acetate extraction, followed by a final purification step using HPLC. 186 Novel and efficient preparation of precursor [188Re(Oh2)3(Co)3]+ for the labelling of biomolecules S.H. Park1, H.J. Gwon1, S.H. Jang1, K.B. Park1, S. Seifert2, H.-J. Pietzch2 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Application, Daejeon, Korea 2Forschungszentrum Rossendorf, Institute of Bioinorganic and Radiopharmaceutical Chemistry Dresden, Germany

The 99mTc(I) and 188Re(I) tricarbonyl precursors [M(OH2)3(CO)3]+ have been shown to be excellent starting materials for the synthesis of further 99mTc(I) and 188Re(I) tricarbonyl complexes as well as radiolabelling of target specific biomolecules [Alberto, R. et al., J. Am. Chem. Soc. 120 (1998) 7987]. Recently, a user-friendly kit formulation (IsoLinkTM) was developed using potassium boranocarbonate, K2[BH3CO2], for preparation of the 99mTc precursor complex. This solid reagent serves both as a source of CO as well as a reductant for technetium. It was also used by Schibli and co-workers for the preparation of the corresponding 188Re precursor complex [Schibli, R. et al., Bioconjugate Chem. 13 (2002) 750]. [188Re]perrhenate eluate (1 ml) was reduced in neutral solution with 3 mg K2[BH3CO2] and 5 mg BH3NH3 by incubation at 60°C for 15 min. The amount of reducing agents and acid (concentrated phosphoric acid) was carefully balanced, to avoid fast hydrolysis of the boranes and to maintain a sufficient low pH to stabilize reduced rhenium intermediates. The preparations resulted in yields >85 % of the desired precursor complex, remaining perrhenate (7±3 %), colloidal 188ReO2 (<5 %), and a byproduct of unknown composition. To overcome the moderate yields we used the recently described borohydride exchange resin (BER) as an additional reducing agent [Park, S. H. et al., J. Labelled Compd. Radiopharm. 47 (2004) 683]. Optimal yields of the precursor complex were obtained using the following preparation conditions: To a vial containing a mixture of 3 mg K2[BH3CO2], 3 mg BH3NH3, and 3 mg BER, 1.0 ml of [188Re]perrhenate eluate and 8 µl phosphoric acid (85 %) were added. The vial was incubated at 60°C for 15 min. Pressure from the evolving H2 gas was balanced with a 20 ml syringe. 90-95 % of the desired 188Re(OH2)3(CO)3]+ complex were found by HPLC and TLC analyses. The assay for the formation of the 188Re(I) tricarbonyl precursor, reduced hydrolyzed 188Re, and [188Re]perrhenate was achieved by investigating their positions using an instant thinlayer chromatography (silicagel//MeOH/HCl (95/5). 188Re(I) tricarbonyl precursor: 90-95% (Rf = 0.4); reduced hydrolyzed 188Re: less than 3 % (origin); [188Re]perrhenate ion: 5-8 % (Rf = 0.8). The identity of the precursor was confirmed by reaction with histidine. The retention time of 188Re(I) tricarbonyl histidine was compared to that of 99mTc(I) tricarbonyl histidine and found to be identical. 187 Radiolabelling of dota-tate with 177Lu. Preliminary studies with a view to somatostatin receptor radionuclide therapy V. Lungu1, D. Niculae1, L. Danaila2, M. Purice3 1National Institute for Physics and Nuclear Enginee, Radiopharmaceuticals, Bucharest, Romania 2Institute of Cerebro-Vasculary Diseases, Surgery, Bucharest, Romania 3Institute of Endocrinology, Nuclear Medicine, Bucharest, Romania This study describes the radiolabelling method of DOTA-TATE with 177Lu as well as the in vitro experiments for quantification of the biological properties. The radiolabelling was performed taking into account the usual biological and radioactively therapeutic doses. Radiochemical purities higher than 95% were obtained for the following parameters: 177Lu to DOTA-TATE molar ratio: 3.8; pH: 4.5 in acetate buffer; incubation time: 30min; temperature: 80°C; HABA (3hydroxi-4aminobenzoic acid) as stabilizer. The competition binding assay of natLu-DOTA-TATE/125I-Tyr3-Octreotide and the saturation binding assay of 177Lu-DOTA-TATE using rat brain cortex membrane as somatostatin receptor model were done. The obtained results, analyzed using Prism 2 software, allow determination of IC50 (4.74 nM) and Kd (142.8 pM). These pharmacological parameters values illustrate the excellent capacity of 177Lu-DOTA-TATE to bind to somatostatin receptors as well as the formed bounds stability. 188 Synthesis of stable isotopically labeled isoflavans T. Jokela, K. Wähälä University of Helsinki, Department of Chemistry, Helsinki, Finland Isoflavans are phytoestrogen derived mammalian metabolites. They are proposed to have even more biological properties such as

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anticancer activity than their precursor isoflavones. The most efficient method to quantify metabolic compounds of isoflavones in biological samples is ID-GC-MS-SIM. Polydeuterated reference compounds are needed as internal standards in quantitative measurements. The reference compound should contain no D0 or D1 species, and there should be a sufficient number of D labels to overcome the overlap in the mass spectrum of M+1, M+2 etc. We have now developed an expedient way to prepare non-aromatically labeled stable D4-isoflavans in excellent yields and isotopic purities over 95%. 189 Development of 111In-DTPA-Human Polyclonal Antibody Complex for Inflammation/Infection Detection A.R. Jalilian, P. Rowshanfarzad, K. Shafaii, M. Kamali-Dehghan, J. Moafian, M. Akhlaghi, M. Babaii, M. Mirzaii, S. Moradkhani, M. Mostaan, F. Saddadi, M. Pooladi Cyclotron & Nuclear Medicine Dept., Nuclear Research Center for Agriculture & Medicine (NRCAM), Atomic Energy Organization of Iran (AEOI), Karaj, Iran Human polyclonal antibody (HIgG) was successively labeled with 111In-indium chloride after residulation with freshly prepared cyclic DTPA-dianhydride. The best results of the conjugation were obtained by the addition of solid DTPA-dianhydride (0.1-0.3 mg) to 100 µl of the HIgG solution (0.2-0.4 mg/ml) at pH=6 in phosphate buffer media at 25°C with continuous stirring for 30 min. Radio-thin layer chromatography showed an overall radiochemical yield of 96-99% at the optimized conditions (specific activity=300-500 MBq/mg, radiochemical purity >98%). Preliminary long-term in vivo studies in terpentine-oil induced inflammation in rat model performed to determine complex distribution of the radioimmuno-conjugate. The target/non target and target-blood ratios were 37 and 51 after 48 and 110h respectively, showing the high selectivity of the radiopharmaceutical for the inflammatory lesions. Posters (T3/S1) 190 Carbon isotopes in soils and lacustrine sediments in paleovegetation and paleoclimate studies during the Holocene in the Southeastern Brazil S.E.M.G. Saia1, L.C.R. Pessenda1, A. Sifeddine2, S.E.M. Gouveia1, J.A. Bendassoli3, I. Karmann4, P. Amaral4 1CENA/USP, C-14 Laboratory, Piracicaba, Brazil 2IRD, Paleotropic Geochemistry, Bondy, France 3CENA/USP, Stable Isotope Laboratory, Piracicaba, Brazil 4USP, Geociences, São Paulo, Brazil This work intends to develop a comparative study in the Atlantic forest located in the south of São Paulo State, involving geochemistry and pollen analyses of lacustrine sediment and carbon isotopes of soil organic matter (SOM). This integration of techniques and researchers must improve significantly the studies of reconstruction concerning vegetation and climatic changes, that occurred in the late Holocene in the southeastern Brazil. The soil samples were collected by drilling in 3 forested points (IPO 1, IPO-LG and IPO-Tatu) up to 350 cm soil depth. In this paper we present the isotope results for the first 50 cm soil depth, which corresponds to approximately the last 1000 yrs BP (with basis on more than 50 radiocarbon dating of humin fraction obtained in different sites in Brazil). A 170 cm depth sediment core was collected with a Vibracorer from an area close to the center of the Lagoa Grande. A chronologic framework for the sedimentary sequence was provided by 5 accelerator mass spectrometer (AMS) radiocarbon dates. In IPO 1, LG and Tatu the C-13/C-12 of shallow soil layer (0-10 cm) of -25.9‰, -28.3‰ and -27.3‰, respectively, characterized the forested vegetation cover. A small C-13/C-12 depletion was observed in all locations up to 50 cm, varying to -25.8 ‰, -26.8‰ and -26.7‰, respectively. These results indicates the dominance of C3 plants in the period and the C-13/C-12 depletion observed is probably due to the isotope fractionation of the SOM decomposition. The TOC and TON concentrations varied in the sediment core from 7% to 2% and 0.9% to 0.05%, respectively and

the C/N ratio of 10 up to 18. The C-13/C-12 values varied through the sediment column between -18‰ and -30‰, probably reflecting changes of input and quality of sedimentary organic matter sediment linked to surroundings vegetation and the organic matter production from the sediment basin associated to lake level variations. N-15/N-14 values around +0.38atoms% indicated the presence of land plants (probably C3 plants) in most of the sediment core, excepted in the layer 120 to 140 cm that presented more depleted values (+0.35atoms%), more enriched C-13/C-12 data (-18 ‰) and higher C/N (~18). Considering these data and the C-14 dating obtained for this layer, a more significant presence of C4 grasses, probably associated with a dry climate, occurred around 680 yrs BP ± 80. A dry episode was observed in the Amazon and other Brazilian regions in similar period (~700 yrs BP). 191 Multi-element determination of El-Rubshi Chromite from Eastern Desert Egypt by Instrumental Neutron Activation Analysis A. El-Taher1, M.A. Khairy2, A.S. Abdel-Halim3 1Faculty of Science, Al-Azhar University, Physics Department, Assuit, Egypt 2Faculty of Science, Almnofia University, Physics Department, Sheben Elkom, Egypt 3Hot Laboratories Center, Radioactive Environmental Pollution, Egyptian Atomic Energy Authority, Cairo, Egypt Neutron activation analysis (NAA) is one of the most powerful analytical techniques for multi-element determination of rocks. In the present work NAA and HPGe detector -spectroscopy was used to determine chromium and 15 minor and trace elements qualitatively and quantitatively from chromite rock samples collected from El-Rubshi area in the Eastern Desert-Egypt. The samples were properly prepared together with their standards and simultaneously irradiated by thermal neutrons at the TRIGA Mainz research reactor. Short time irradiation (1-5 min) were used to determine Mg, Ti and Mn. Long time irradiation (6 hours) were used to determine Na, Ga, As, La, Sc, Cr, Fe, Co, Zn, Zr, Ce, Yb, Lu, Hf and Ta. In El Rubshi chromite comprises 18 sites, more than 100 lenses of massive chromite, more than 2700 tons averaging 44 % Cr2 O3 and the average of 51Cr is 40.2 %. 192 Palaenvironmental reconstruction (vegetation and climate) in the northeastern region of Brazil during late Pleistocene and Holocene using carbon isotopes of soils S.E.M. Gouveia1, L.C.R. Pessenda2, A.S. Ribeiro3, R. Aravena4, J.A. Bendassolli5, S.E.M.G. Saia2, M. Vedoveto2 1Centre for Nuclear Energy in Agriculture, C-14 Laboratory, Piracicaba, São Paulo, Brasil 2University of São Paulo, CENA- Radiocarbon Laboratory, Piracicaba, Brazil 3Federal University of Sergipe, Department of Biology, Aracaju, Brazil 4University of Waterloo, Department of Earth Sciences, Waterloo, Canada 5University of São Paulo, CENA - Stable Isotope Laboratory, Piracicaba, Brazil This paper presents the first results on a research project that has the objective to expand the palaeoenvironmental studies (vegetation and climate) for the Northeastern region of Brazil in the last 15,000 years. Samplings have been made in three states of the region (Piauí, Ceará and Paraíba). Soil profiles were sampled for C-13/C-12 analysis, as well as buried charcoal fragments were used for C-14 dating. In the area of Parque Nacional Sete Cidades (Piauí State) the isotope enrichment trend from -24.2‰ to -19.1‰ observed during early-mid Holocene is an indication of opening of an arboreal (woody savanna) vegetation (probably associated with the expansion of C4 plants) and a trend toward -26.5‰ observed in the late Holocene indicated the dominance of C3 plants. A similar trend is observed at Floresta Nacional do Araripe (Ceará State) and Reserva Biológica Guaribas (Paraíba State) where values of ca. -24.0‰ and -21.0‰, respectively, indicate the presence of woody savanna during late Pleistocene. In the early-mid Holocene more

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enriched values (up to -18.0‰) suggest a more significant presence of C4 plants. The presence of buried charcoal fragments in several depths of the soil profiles suggested the occurrence of paleofires during the Holocene, reinforcing the dry early-mid-Holocene period. Based on the isotopic data obtained, it is possible to postulate that approximately since the late Pleistocene (~15,000 yr B.P) to the early Holocene (~10,000-9000 yr B.P), arboreal vegetation comprising of forest and woody savanna was present in the study areas. This phase was probably related to a more humid phase. Afterward, since ~9000 yr BP till 4000-3000 yr BP, the woody savanna expanded, probably related to the presence of a drier climate. The charcoal presence at the study sites confirms the occurrence of a dry phase during this period. From approximately 4000-3000 yr BP to the present, a trend toward more depleted values was interpreted as an arboreal vegetation expansion due to the return to a more humid phase and probably similar to the present climate. These results agree with studies developed in other regions of the NE Brazil and also in the south and central Amazon region, implying that similar climatic conditions have affected these areas during the late Pleistocene until the present. Posters (T4/S2) 193 An evaluation of the radiation dose distribution in a Co-60 irradiation chamber using chemical dosimeter, TLD and ionization chamber J. Park1, Seong-Ae2, Moon2 1Cheju National University, Applied Radiological Science Research Institute, Jeju-si, South Korea 2Cheju National University, Nuclear & Energy Engineering, Jeju-si, South Korea The radiation dose distribution inside the panoramic irradiation chamber with a Co-60 gamma source of 400 TBq(20,800Ci), which is located at Applied Radiological Science Research Institute of Cheju National University in South Korea, is evaluated using a chemical dosimeter, a thermoluminescence dosimeter (TLD), and a Farmer-type ionization chamber. The chemical dosimeter is made with a FeSo4 solution and the TLD is consists of CaSO:Dy TL pellets manufactured in Korea Atomic Research Institute. The absorbed dose is measured at a number of distances from the source as well as by applying different thicknesses of lead shielding. The lead shielding consists of three cylindrical layers of the same thickness, which can wrap around the source rod one after another. It is assumed that the ionization chamber should produce the most accurate results. The results measured with the chemical dosimeter and the TLD are compared with those obtained with the ionization chamber to estimate the accuracy of the former two dosimeters at high absorbed doses. The limitation of the TLD and chemical dosimeter in measuring high radiation doses is discussed. The effects of the lead shields and the distance between the source and the dosimeters on reducing the doses are analyzed. The dose distribution curves which take into account the effects of the distance and the lead shields are presented. 194 Radiation related gene expression in mutants of Bacillus lentimorbus WJ5 induced by gamma-radiation (60co) Y.-S. Jang, Y.-K. Lee, H.-H. Chang, H.-Y. Chung Korea Atomic Energy Research Institute, Radiation Application Research Division, Yuseong, Daejeon 305-353, South Korea Ionizing radiation, such as γ-radiation, has a clear mutagenic potential inducing many different types of DNA damages. In order to study the expression of the radiation related genes in mutants induced by gamma radiation, the simultaneous gene expression was analyzed by DNA microarray. Mutants of B. lentimorbus WJ5 were induced by 60Co γ-radiation at the dose of LD95 (3.8 kGy). We constructed DNA chips including two thousands of randomly digested genome spots and compared its quantitative aspect with seven mutants (WJ5m4, WJ5m12, WJ5m16, WJ5m35, WJ5m42, WJ5m63, and WJ5m86). From the cluster analysis of gene expression pattern, totally 408 genes were expressed and 27 genes

were significantly upregulated by the gamma radiation in the above all mutants. Especially, genes involved in DNA repair (mutL, mutM), energy metabolism (acsA, sdhB, pgk, yhjB, citB), protease (npr), and reduction response to oxidative stress (HMM) were simultaneously upregulated. It seems that the expression of the repair and resistance related genes in mutants induced by γ-radiation could be remarkably different from that of acute exposure. 195 Improvement of the wear resistance of ultra high molecular weight polyethylene (UHMWPE) by radiation cross linking Y.C. Nho, P.K. Kang, S.S. Kim Korea Atomic Energy Research Institute, Radiation Application Division, Daejon, Korea The effect of thermal treatment and irradiation on the physico-chemical properties of ultra-high molecular weight polyethylene (UHMWPE) used in orthopedic implants was investigated. If a large amount of polymer radicals remain trapped after the irradiatino of ultra-high molecular weight polyethylene (UHMWPE), the radicals may result in a significant alteration of its properaties during shelf storage and implantation for a long time period. An electron spin resonance spectroscopic study was undertaken to investigate the remaining free radicals in IHMWPE after irradiation in air and a N2 environment. Heat treatment was employed for various periods of time to scavenge the free radicals. The heat treatment of irradiated UHMWPE could substantially reduce the concentration of the free radicals; therefore the long-term oxidative degradation of UHMWPE was reduced. The surface oxidation on the UHMWPE samples according to irradiation and the thermal treating condition was verified by FTIR-ATR and electron spectroscopy for chemical analysis (ESCA). The polymer pin on metal plate type testing apparatus was used to test wear property. UHMWPE irradiated in the molten state had a higher crosslinking extent and a lower wear rate than one irradiated in the room temperature. 196 Improvement of melt strength of polypropylene by radiation P.H. Kang, Y.C. Nho Korea Atomic Energy Research Institute, Radiation Application Division, Daejon, Korea In the present study, the effects of radiation and addition of polyfunctional monomer on the melt strength of polypropylene (PP) were investigated. Polypropylene (PP) has been widely used in industrial applications because of its various excellent properties such as a high stiffness and good heat and chemical resistance, but its linear structure leads to poor processibility in processing involving melt strength, such as extrusion coating, foam extrusion and film blowing. To improve melt strength, the PP films were prepared by blending with poly functional monomer (PFM) such as 1,4 butanediol dimethacrylate and diethyleneglycol dimethacrylate. The concentration of the polyfunctional monomer was below 3 parts per hundred resin(phr). The irradiation was conducted from 1kGy to 100kGy in nitrogen. Following irradiation, the PP specimens with polyfunctional monomer were thermally treated at 160 centi degree to eliminate all the remaining free radicals. The melt strength of the irradiated PP was measured by tensile tester for polymer melts (Rheotens, Göettfert GmbH, Germany) at 210 centi degree. Dynamic mechanical analysis and tensile property of these irradiated specimens have been investigated as well. 197 The gamma irradiation of microstructure and physical property of polypropylene P.H. Kang, Y.C. Nho, S.M. Lee Korea Atomic Energy Research Institute, Radiation Application Division, Daejon, Korea The effects of thermal treatment after radiation on microstructure and physical property of polypropylene (PP) were investigated. Isotactic PP(i-PP) was selected as the polymer matrix in this work. The PP sheets were prepared by pressing into a 1mm sheet at 200 centi degree. Co60 gamma ray irradiation was conducted at 25kGy

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in nitrogen. Following the irradiation, the PP sheet was thermal-treated at various temperature to remove the remaining the radicals. The microstructure of i-PP such as crystalline phase, before and after thermal treatment after irradiation was evaluated by WAXD (wide angel x-ray diffraction). The crystallinity of the samples was evaluated, by differential scanning calorimetry (DSC), from the heat of fusion relative to a value of 209 J/g corresponding to a 100% crystalline PP. Thermal property of the i-PP after irradiation was also analysed by DSC. Tensile property of these irradiated specimens have been investigated as well. 198 Radiolysis of polytetrafluoroethylene and polystyrene catalytic suports in presence of tritiated water C. Postolache, L. Matei, V. Fugaru, N. Negoita National Institute for Physics and Nuclear Enginee, Radioisotope Production Centre, Bucharest, Romania The behavior of hydrophobic catalyst supports in the isotopic exchange reactions H/D/T was analyzed by determination of self radiolytical processes in presence of tritiated water. In this study, was analyzed the behavior of polytetrafluoroethylene and styrene-divynil benzene copolymer catalyst supports in presence of tritiated water. Self radiolytic effects were evaluated using quantum-chemical methods. The primary radiolytic effect was analyzed using a two-step radiolytic mechanism: a) ionization of molecule and spatial redistribution of atoms in order to reach a minimum value of energy, characteristic to the new quantum state; b) neutralization of molecule by capture of an electron and its rapid dissociation in free radicals. Chemical bonds suspected to break are located in the distribution region of LUMO orbital and have minimal binding energy. Evaluation of secondary effects which happens in water presence in polymeric structure was carried out through, by studying the transition state resulted after the attack of HO• radicals formed by tritiated water radiolysis. Radiolytical processes were analyzed by catalytic supports immersed in deuterated water exposure at gamma field radiation emitted by a 60-Co source. After that, were performed the analysis of chemical modification by IR spectroscopy, GC MS and hydrofluoric acid emission, in case of PTFE. Catalytic supports were exposed at tritiated water with a high specific activity and residual activity was determined. Obtained results by quantum-chemical simulation were compared with experimental results. 199 Engineering applications of hydrophobic pt-catalysts in nuclear field I. Popescu, G. Ionita, C. Varlam, I. Stefanescu ICIT Rm. Valcea ROMANIA, Isotopes Laboratory, Rm. Valcea, Romania Based on the long experience of the authors, in the preparation, testing and evaluation of the performances of hydrophobic catalyst, and based on the reviewed references, this paper presents up-to-date R&D activities on the application of the hydrophobic Pt catalysts, in deuterium and tritium separation separation from nuclear effluents. Unlike the conventional hydrophilic catalysts, the hydrophobic catalysts kept a high catalytic activity and stability, even under the direct contact to liquid water or in presence of saturated humidity. A large diversity of catalyst types (over 100 catalysts) was prepared and tested in order to make feasible the hydrogen isotopes separation processes. The enrichment of deuterium and tritium by isotopic exchange between water and hydrogen, tritium removal from heavy water reactor and nuclear reprocessing plant, the cleanup of atmosphere and gaseous effluents by catalyzed hydrogen-oxygen recombination, are largely presented and discussed. The objectives of the work are: (1) to provide a database for selection of the most appropriate catalyst and catalytic packing for above mentioned process, (2) the designing and operation reactor packed with hydrophobic catalysts, (3) to evaluate the potentiality of hydrophobic Pt-catalysts in the deuterium and tritium enrichment. The merits of the hydrophobic catalyst are

shown in comparison to hydrophilic catalyst. Some suggestions concerning the deuterium and tritium enrichment by means of hydrophobic catalyst are also discussed. Posters (T5/S1) 200 Electrochemical deposition of I-125 from alkaline solutions on silver substrate N.A. Nerozin, V.V. Kanygin, D.A. Podsoblyaev, A.A. Raspopov, B.B. Shapovalov, E.Ya. Smetanin, N.A. Melnichenko, M.V. Gevorkyan SSC RF - IPPE, Institute of Isotopes and Radiopharmaceuticals, Obninsk, Russia Brachytherapy currently finds wide spread application for prostate cancer therapy. This method proposes the insertion of several tens of seeds based on I-125 or Pd-103 isotopes into the patient's prostate, and radiation of these seeds destroys the tumor. In this case I-125 is deposited on silver wire, which is enclosed with titanic case (this is one of possible designs of seed-implantate). Iodine should be deposited on silver in the form of strong layer. There are several methods of iodine deposition on noble metals: substitution (isotopic and non-isotopic) and electrochemical deposition. I-125 electrochemical deposition on silver exceeds substitution method in its parameters (formation of strong dense layer on a surface, uniformity of layer, quantity of isotope deposited, possibility of rated deposition). Methods of substitution and electrochemical deposition have been tested and work in neutral and subacid solutions (3 < pH < 8). However, operations with solutions containing radioactive iodine do not exclude I-125 vapor ingress into atmosphere. Since I-125 ingress into atmosphere is undesirable two ways of solving the problem exist: 1. Use of leak-tight facilities and scrubbers-absorbers. 2. Deposition directly from alkaline solutions. In addition to simplicity of needed equipment the second way has one more advantage: deposition is carried out directly from process solutions (0.05M NaOH) without additional operations. This report is devoted to the possibility of such deposition. 201 Influence of iron deficiency in the labeling of red blood cells with 99mTc G.P. Calmanovici1, M.J. Salgueiro1, N.M. Leonardi1, C.G. Goldman1, J.R. Boccio2, M. Zubillaga1, 1Radioisotope Laboratory, Physics Department, School of Pharmacy and Biochemistry, University of Buenos Aires, Buenos Aires, Argentina 2School of Pharmacy and Biochemistry, University of Buenos Aires, Physics Department, Buenos Aires, Argentina Introduction: red blood cells (RBCs) labeled with 99mTc are commonly used in the evaluation of cardiac function, gastrointestinal tract bleeding, red blood cell volume or splenic sequestration. Generally stannous ion is used as reducing agent. A proposed mechanism is that once the stannous ion (Sn) and the pertechnetate (99mTc) reach the interior of the RBC, the radionuclide is mainly house in the b-chain of hemoglobin. The aim of this study is to determine if the diminishing in hemoglobin content affects the RBC labeling efficiency and the biological distribution of this radiopharmaceutical. Materials and methods: we studied three groups of rats fed for 3 weeks after weaning with a diet with an iron content of 6.5 ppm, 18 ppm and 100 ppm, with hemoglobin (7.26 ± 2.5) g/dL, (10.67 ± 0.91) g/dL and (15.58 ± 0.83) g/dL, respectively; defining 3 groups: iron deficient, moderate iron deficient and control. Each rat was intravenously injected with 5 mg of stannous chloride (2.1 x 10-2 mg/kg) and 15 minutes afterwards with 10 uCi of a solution of 9mTcO4-. Blood samples were taken 15 and 30 minutes after the labeling procedure, and the radioactivity in the plasma (AP) and in red blood cells (ARBC) were determined separately to calculate the labeling efficiency. The animals were sacrificed 30 minutes after

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the labeling procedure; extracting blood, spleen, liver, kidneys, stomach, intestines, heart and lungs. The percentage of radioactivity (%A) for each organ was calculated. Results: the labeling yield for the iron deficient, moderate iron deficient and control groups for 15 minutes were respectively 98.12% ± 0.22 %, 98.25% ± 0.68% and 98.93% ± 0.16%; and for 30 minutes was respectively 98.53% ± 0.56%, 98.45% ± 0.62% and 99.34 ± 0.43%, without statistical differences among groups and between times. In the biological distribution studies, the percentage of radioactivity for the iron deficient, moderate iron deficient and control groups was mostly founded in blood (74.65% ± 5.21%, 70.57 ± 9.50% and 68.86% ± 7.05%, respectively). The radioactivity founded in the rest of the studied organs was almost negligible. Even though, no difference among groups was observed in each studied organ. Conclusions: the iron deficiency does not interfere neither in the labeling nor in the biodistribution of the red blood cells labeled with 99mTc. 202 An application of Holmium-166-Chitosan complex to an oral cancer therapy B. Shin1, J.Y. Paeng2, S.J. Kim1, S.M. Choi1, S.H. Park1, H.J. Gwan1, M.J. Kim2 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Daejeon, Korea 2Seoul National University, College of Dentistry, Seoul, Korea Radiation therapy has been used for the oral cancer treatment as a main treatment modality. The purpose of this study was to evaluate the effect of Ho-166-chitosan complex could be applied to the oral cancer therapy. The KB cell line was injected into the flank of the athymic mice and at the injection site the human oral cancer was induced. In those animal model, it was measured the organ leakages of radioisotope and the tumor size after intratumoral injection. The major organs of the mice injected with the Ho-166-chitosan complex showed much lower radioactivity than those of the mice with the Ho-166 alone. The sum of the radioactivity in major organs at 24 hours after the intratumoral administration was 0.01 ± 0.001 %ID/g for the Ho-166-chitosan and 0.70 ± 0.102 %ID/g for the Ho-166 alone. The tumor size was decreased until three weeks in the Ho-166-chitosan complex injected group but in the control group the tumor grew up. The tumor volume of Ho-166-chitosan was 7.4 times smaller than the control group. The above data suggested that most of the Ho-166-chitosan complex is retained in the injected site and the complex suppress the tumor growth. Thus the complex represents a promising candidate for oral cancer therapy. 203 Brachytherapy of squamous cell carcinoma in cats using a 32P patch M.J. Salgueiro1, M. Soberano2, J. Nicolini3, R. Ughetti3, M. Nicolini3, M. Zubillaga1 1Radioisotope Laboratory, School of Pharmacy and Biochemistry, University of Buenos Aires, Physics Department, Buenos Aires, Argentina 2Centro de Radioterapia para Animales de Buenos Aires (CRABA), Veterinary, Buenos Aires,Argentina 3Laboratorios Bacon SAIC, Buenos Aires, Argentina Brachytherapy, that is, the placement of radioactive sources into or near the tumor, has been a big challenge in nuclear medicine for the therapy of cancer. Our group has been studying unsealed B-negative sources for oncological therapeutic purposes during ten years. PirocarbotratTM, is a gelatin-protected charcoal suspension labeled with chromic [32P] pyrophosphate that behaves very much like a sealed B- radiation source for the treatment of solid tumors. The aim of this work was to make use of these properties in order to design a silicon patch coated with PirocarbotratTM for topical application in skin cancer lesions. For this purpose, we selected four adult cats with nasal, state II squamous cell carcinoma (SCC). Measurements of the lesions were taken and the patches were specially designed for its application on the lesion surface with minimal contact with the normal surrounding tissue. Animals were

then anesthetized to get inmobilized to both facilitate patches application and to prevent their remotion. Dosimetric calculations were done in each case taking into account the time of exposure and the activity contained in the patch. Total surface of the patches was 4.5 cm2 and the activity per surface varied between 30.7 - 32.2 MBq (871.3 - 830.1 uCi / cm2). The patches were applied on the surface of the nose SCC lesions for 3.5 - 4.0 hours for a total radiation dose of 28 - 33 Gy (2800 - 3300 rads). During the time of exposition, the animals were isolated in cages specially conditioned for this purpose. When exposing time finished, the patches were removed and the animals were returned to their owners. The first post-treatment control visit was planned to be fifteen days after patch application. Until now, we could only evaluate one of the four treated cats. In this case, clinical evaluation showed that the tumor disappeared and an erythema with alopecia and hypopigmentation developed in the treated site. We took samples to perform the follow-up biopsy and we are expecting histopathology results. With regard to the other three treated cats, we are still waiting the first post-treatment period to pass in order to be evaluated in the same way. Follow-up controls of all the four cats will be performed up to one year or until possible recurrences will be detected. 204 Magnetic resonance and nuclear imaging combined with therapy of tumours using 166Ho-loaded particles J.F.W. Nijsen1, G.C. Krijger2, S.W. Zielhuis1, G.A. Koning2, J.H. Seppenwoolde1, M.A.D. Vente1, C.J. Bakker1, R. de Roos1, B.A. Zonneberg1, A.D. van het Schip1 1University Medical Center, Nuclear Medicine, Utrecht, The Netherlands 2Delft University of Technology, Radiation, Radionuclides and Reactors, Delft, The Netherlands Introduction: Cancer treatment with holmium-166 (166Ho) has numerous advantages over other radionuclides for therapeutic purposes, since holmium is the only element which can both both be neutron-activated to a beta- and gamma-emitter with a logistically favourable half-life, and be visualised by MRI (165Ho, 100% natural abundancy) [1]. Because the chemical properties of all lanthanides and some other elements are similar to those of holmium it will be relatively easy to produce systems adapted for specific treatment/diagnostic demands based on the knowledge of holmium-loaded systems. For treatment of unresectable liver tumours internal radiation therapy is thought to be a promising alternative [2]. During this therapy 166Ho containing poly(L-lactic acid) microspheres (PLLA-MS) are administered into the hepatic artery. These microspheres will lodge in and around the tumour and irradiate the surrounding tissue. Recently, promising results have been obtained with 166Ho-loaded PLLA-MS in rats [3]. In addition, initial studies using holmium containing liposomes for detection and imaging of lymph node and/or lymph node metastases around malignancies like breast tumours were performed. During these studies the value of the combination of MRI and nuclear imaging for therapeutic and diagnostic systems will be explored. Methods: Poly(L-lactic acid) (PLLA) microspheres loaded holmiumacetylacetonate (HoAcAc) are produced by the solvent evaporation technique. These microspheres are graded and collected according to size on stainless steel sieves of 20 and 50 µm [4]. Afterwards the microspheres are irradiated in a thermal neutron facility at the Reactor Institute in Delft. Liposomes were prepared by the conventional thin film hydration technique and contained DTPA-bisoctadecylamide (a lipid coupled to a chelator). The resulting lipid film was subsequently hydrated in an acetate buffer pH 5.5. The resulting lipid dispersion was extruded using polycarbonate membrane filters with a pore diameter of 400 nm and 200 nm combined with 100 nm. The liposomes had a diameter of around 170 nm and were labeled afterwards with 166HoCl3. Both the liposomes and the microspheres were tested in phantom and animal studies. To determine the ability of MRI and nuclear imaging to visualize the in vivo biodistribution of the holmium loaded systems, rats and rabbits were injected with these systems. MR imaging was performed before and after treatment. Tumour size was monitored by ultra sound measurements. All experiments were performed in agreement with the Netherlands Experiments on

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Animals Act (1977) and the European Convention guidelines (86/609/EC). Results and Conclusions: 166Ho-loaded microspheres and liposomes can be produced under reproducible conditions. The systems are stable with and without 166Ho and can be detected with MRI and nuclear imaging in phantom studies (tubes with particles in agar gels). Scintigraphic images of injected 166Ho-loaded microspheres in the hepatic artery showed accumulation of radioactivity in and around implanted liver tumours in rats and rabbits. MRI of treated living rabbits showed the additional value of MR over nuclear techniques: the in vivo biodistribution of the holmium microspheres could be easily visualized, allowing depiction of the microspheres in relation to the tumour and its surroundings. No primary tumour growth was seen in rabbits treated with 900 MBq of activity. Subcutaneously injected liposomes in rabbit feet showed good detection of the first lymph node and reasonable detection of the second one using nuclear imaging. MR imaging did not result in detectable concentrations of liposomes and additional experiments will be performed to result in higher levels of liposome targeting. References: 1. Nijsen JFW, Seppenwoolde JH, Havenith T, Bos C, Bakker CJ, het Schip AD. Liver Tumors: MR Imaging of Radioactive Holmium Microspheres--Phantom and Rabbit Study. Radiology 2004; 231:491-499. 2. Nijsen JFW, van het Schip AD, Hennink WE, Rook DW, van Rijk PP, De Klerk JMH. Advances in nuclear oncology: Microspheres for internal radionuclide therapy of liver metastases. Current Medicinal Chemistry 2002; 9: 73-82. 3. Nijsen F, Rook D, Brandt C, Meijer R, Dullens H, Zonnenberg B, de Klerk J, van Rijk P, Hennink W, van het Schip AD. Targeting of liver tumour in rats by selective delivery of holmium-166 loaded microspheres: a biodistribution study. Eur J Nucl Med 2001; 28: 743-9. 4. Nijsen JFW, Zonnenberg BA, Woittiez JR, Rook DW, Swildens-van Woudenberg IA, van Rijk PP, het Schip AD. Holmium-166 poly lactic acid microspheres applicable for intra-arterial radionuclide therapy of hepatic malignancies: effects of preparation and neutron activation techniques. Eur J Nucl Med 1999; 26: 699-704. 205 The radiation effect of the holmium-166 on various oral cancer cell lines S.J. Kim1, J.Y. Paeng2, K.B. Park3, B.C. Shin1 1Korea Atomic Energy Research Institute, Division of Radioisotope Production and Applications, Daejeon, Korea 2Seoul National University, College of Dentistry, Seoul, Korea 3Seoul National University, Center for HANARO Applications Research, Seoul, Korea Radiation is an effective treatment modality for an oral cancer treatment. Recently an internal radiotherapy using Ho-166 was developed and applied to various cancers, especially a liver cancer. The purpose of this study was to evaluate the effect of Ho-166 on various oral cancer cell lines. The radiation effect of Ho-166 was evaluated by a cytotoxicity assay, a TUNEL assay and a flow cytometry for various oral cancer cells (KB, HSC-3). The radiosensitivity of the oral cancer cell lines was evaluated with a gradual increasing of the radiation activities of Ho-166. Oral cancer cell lines showed a sensitivity to a beta ray from Ho-166 but the degree of the sensitivity was different according to the cell lines. The KB cell was more sensitive to a beta-ray for the MTT assay and a large apoptotic feature was found for the TUNEL assay. From this study, Ho-166 was shown to be a beneficial and effective source, as a brachytherapy agent, for the treatment of oral cancer. 206 Total energy expenditure and physical activity level of Cuban preschoolers measured by the doubly labeled water method M. Hernandez-Triana1, G. Salazar2, E. Diaz-Bustos2, S. Gonzalez-Calderin1, M. De la Paz-Luna1, V. Ruiz-Alvarez1, M.E. Diaz3 1Institute of Nutrition, Biochemistry and Physiology, Havana, Cuba 2INTA, Stable Isotopes Lab, Santiago de Chile, Chile 3Institute of Nutrition, Anthropology Lab, Havana, Cuba The doubly-labelled water method is the most appropriated and widely accepted technique for the assessment of the total daily energy expenditure (TEE) and Physical Activity Level (PAL) of people living in their own environment. Those methods based on

isotope dilution using 2H or 18O are appropriated indicators for the exact measurement of the total daily energy expenditure of subjects living in their own environment. The effectivity of the Cuban Food and Nutrition Program for preschoolers was evaluated by using the comparison of the food energy intake with the TEE measured by this isotopic technique. Additinally, the results of this project were used in efforts to refine the energy requirements of preschoolers and to contribute to the data based of FA/WHO/UNU for this purpose. During 7 days, TEE was registered by the doubly labeled water method in fifty three 4-6 y old Cuban children living in a rural community, in a small town or in a big city of the island. Additionally the time expended in physical activity was measured by alternative methods as heart rate monitoring and Tritracs sensors. The values were compared with the values of the energy intake measured by the 3-days weighed method. Boys or girls of the 3 communities, showed levels of TEE of 86 and 79.4 kcal/kg/d, and PAL values of 1.77 and 1.66 respectively, values which are 20% higher than those of children living in urban settings of industrialized countries. The Cuban children expended 30-40% of the day time in physical activities like playing indoors or running outdoors. Small town and rural children showed a higher TEE and PAL than children from the big city. Their energy intake covered the energy expenditure in values close to 100%. The values of physical activity and activity energy expenditure of the Cuban children do not match the results used by the 2004 Expert Committee on Energy from FAO/WHO/UNU for the proposal of the new daily energy intake recommendation for pre-school children. The higher values of TEE measured by the doubly labelled water method in rural and urban Cuban children living in totally different geographical environments and cultural backgrounds as the children used as references for the new proposals of the recent Expert Committee on Energy support the requirement of further research in other countries of the region with the assistance of the International Atomic Energy Agency. Posters (T5/S2) 207 Drug development in boron neutron capture therapy E. Pasini1, A. Wittig2, W. Sauerwein2 1BPRC, Chemistry and Parasitology, Rijswijk, The Netherlands 2University of Essen, Radiotherapy, Essen, Germany Drug Development in Boron Neutron Capture Therapy (BNCT) is a matter of high importance and of high delicacy. At present, the medium-large pharmaceutical industry has shown little interest in investing in drug development in this field as the therapy has yet to be fully established, the conventional drug development schemes would have to be tailored, new expertise - normally atypical for a pharmaceutical industry - would have to be brought into the house or suitable collaborations would have to be found with entities that have such expertise and only small numbers of patients could be treated with the facilities available at the moment. The on-going clinical trials make use of two drugs developed in the sixties, BSH and BPA, when pharmaceutical standards did not require the systematic drug evaluation, that industries are asked for at present. Such drugs are made available by small-medium industries that concentrate their resources on production, being too small to invest great amounts of money in research. As a consequence of this, the research for new compounds is mostly limited to public institutions such as universities and research foundations, compounds synthesized are not screened further than on cell lines and potentially useful molecules remain confined to someone's Ph.D. thesis, while new drugs are desperately needed and could allow a break-through not only for BNCT but also in cancer therapy in general. Here we present a possible drug development scheme tailored to BNCT around which motivated researchers with different expertise both from industrial and the academic world can be brought together with the common goal of developing new pharmaceuticals for this innovative therapy.

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Posters (T5/S3) 208 Preliminary estimates for the new way of Thorium-229 production for alpha radioimmunotherapy D. Markovskij, D.Y. Chuvilin, Ilyin E.K. RRC "Kurchatov Institute", Nuclear Fusion Institute, Moscow, Russia Radioimmunotherapy using α-emitting radionuclides is the most promising and rapidly developing method of oncology disease treatment. High initial energy of α-particles and their short path in biological tissues (tens of microns) results in a high-level energy release in that tissue. The carriers of α-emitting radionuclides with high specificity allow transporting them precisely in a tumoral knot or metastatic locus. A selective irradiation of pathological objects with minimum damage to surrounding healthy tissue is possible. When considering the nuclear-physical, chemical, and biological parameters, the most promissing α-emitting radionuclide is 213Bi (T½=45.6 min). 213Bi is the product of the decay chain of 229Th, which could be a product of 233U remaining in nuclear waste. The 213Bi precursor in a decay chain is 225Ac with a half-life period of T½ =10.0 d. For reception of 213Bi, the 229Th/225Ac/213Bi generator system is to be created. Therefore, in the long-term prospect of generating α-emitting radionuclides the process of 229Th reception, as a starting material, is of key importance. A few ways of 229Th and 225Ac reception are known: by radiochemical separation from aged storages of 233U; by photoneutron reaction 226Ra (γ,n)225Ra→225Ac on linac; as a result of multiple neutron capture in a high flux a reactor by the reaction 226Ra(3n,2β)229Th→225Ra→ 225Ac. Unfortunately, the storages of aged 233U are limited, and the use of 226Ra involves numerous ecological problems. Therefore searching of alternate variants of 229Th production remains an actual problem. The proposed method of 229Th production in significant amounts is based on use of 230Th (Iionium (Io), T½=75 thousand years), a natural radionuclide of uranium family in content of 18 grams per ton of uranium. Significant amounts of 230Th are accumulated in storage of the enrichment industry during manufacture of enriched 235U. The possibility of commercial producing 229Th for medical use by irradiation of 230Th targets in fast reactors, cyclotrons and linacs is of greatest interest. Preliminary estimates show that reasonable quantities of 229Th might be produced at existing nuclear facilities using following reactions: 1) Irradiation of 230Th in fast reactors, 230Th(n,2n)229Th reaction. 2) Irradiation of 230Th by protons in cyclotrons, 230Th(p,pn)229Th and 230Th(p,2n)229Pa→→Th reaction. 3) Irradiation of 230Th by γ-rays, Bremsstrahlung generated in an linac, 230Th(γ,n)229Th reaction. Posters (T5/S4) 210 Highly efficient automated synthesis of [11C]choline J. Zhang1, J. Tian1, B. Chen2, Z. Guo1 1The PLA General Hospital, PET Center, Beijing, China 2Center Hospital of Jing Zhou, Dept. of Nuclear Medicine, Beijing, China Objectives: radioactively labeled choline is considered to be a marker for assessment of malignant transformation and proliferation by non-invasive methods such as PET. The production of [11C]-Choline procedure should be well suited for an easy automation with a minimization of residual content of 2-(dimethylamino)-ethanol (DMAE), as it may compete with the uptake of [11C] choline into the cell although DMAE is non-toxic and used as nutrition additive. So we reported a method with 1mg precursor for highly efficient automated synthesis of 11C-choline. Methods: the [11C]-methyl triflate which was translated from [11C] methyl iodide, was bubbled to a reaction vessel tube (1 mg DMAE dissolved in 50 ml acetone, and cooled with ice/water bath, measured in a dose calibrator). While warming to room

temperature. Afterwards, the reaction vessel was washed with 10 ml of ethanol directly, and 11C-Choline was delivered to the cation exchange cartridge (CM). The CM cartridge was washed with 10 ml of water and then the purified [11C] choline was eluted by 5 ml 0.9% NaCl and measured in a dose calibrator. Results: [11C] choline was synthesized in a very simple method by labeling very small amounts of DMAE at rt. with [11C]-methyl triflate. The reaction was optimized concerning amount of precursor. The radiochemical yields increased with increasing amount of precursor. A plateau was reached with 1 mg of DMAE at 97% (EOB with methyl triflate). With the method, we can get 3.7 GBq with irradiations of 40mA beam current and 5 min irradiation time, radiochemistry purity more than 98% and residual DMAE could be kept at a minimum in the product solution. So far many methods of radiosyntheses of [11C]choline have been published. Most of them, [11C]methyliodide was reacted with 100 - 500 ml (the least was 60 ml) of DMAE at rt. or aboven 100 C°, then the product was purified using solid phase extraction cartridges with a cation exchange resin. High of precursor, high residual content of DMAE in [11C]choline. DMAE is of little toxicity, but may metabolically interfere with [11C]choline and disturb uptake of (11C)choline if the injected quantities are high. Conclusion: [11C] choline was synthesized with 1mg DMAE in a radiochemical yield up to 97% (EOB). The content of the precursor DMAE in production was very low. 211 Preparation of [61Cu] Pyruvaldehyde-bis(N4-methylthiosemi-carbazone complex as a possible PET radiopharmaceutical A.R. Jalilian1, M. Ensaf, P. Rowshanfarzad1, M. Sabet2 1Cyclotron and Nuclear Medicine Department, Nuclear Research Center for Agriculture & Medicine, Atomic Energy Organization of Iran, Karaj, Iran 2SSDL and Health Physics Department, Nuclear Research Center for Agriculture and Medicine, Atomic Energy Organization of Iran, Karaj, Iran Copper-61 (T½=3.33h) produced via the nat.Zn(p,xn) 61Cu nuclear reaction using natural zinc target was separated from the irradiated target by a two-step method developed in our laboratory and was used for the preparation of [61Cu]-pyruvaldehyde-bis(N4-methylthiosemicarbazone) ([61Cu]-PTSM) using an in house-made PTSM ligand. An electroplated natural zinc layer on a gold-coated copper backing (zinc and gold layer thicknesses were 80 and 50 µm respectively) was irradiated with 22 MeV protons (22-12 MeV on the target). 61Cu was separated by a two-step column chromatography method using a cation and an anion exchange resin column which gave satisfactory results. After 150 µA irradiation of the target for 76 minutes, about 6.33 Ci of 61Cu2+ was obtained with a radiochemical separation yield of more than 95% and a radionuclidic purity of more than 98%. 64Cu was the only radionuclidic impurity in the separated 61Cu2+ solution. Colorimetric methods showed that traces of chemical impurities in the product were below the accepted limits. The solution of [61Cu]-PTSM was prepared with a radiochemical yield of more than 80%, radiochemical purity of more than 98% and specific activity of about 246 Ci/mmol. 212 The preparation of selective Cox-II inhibitor via nucleophilic fluorination and biological study G. An, K.S. Chun, C.W. Choi KIRAMS, Cyclotron application, Seoul, Korea Objective: In these day, NASIDs (non-steroidal anti-inflammatory drugs) such as aspirin, diclofenac and ibuprofen are the most common medications used to reduce pain and inflammation. However, they act by inhibiting both COX-I and COX-II which can cause serious gastrointestinal side effects such as ulcers, stomach perforations and bleeds. COX-I produces prostaglandins believed to be responsible for the protection of the stomach lining. However, COX-II produces prostaglandins believed to be responsible for pain and inflammation. Recently, the most widely studied selective COX-II inhibitor such as celecoxib and rofecoxib' one work by inhibiting the effect of COX-II on pain and inflammation without

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inhibiting COX-I which protects gastrointestinal lining. Especially, the isoxazolyl compounds have little side effects and the effects of them are known already. Method: We prepared COX-II inhibitor which has isoxazolyl ring. The synthetic route for precursor employed deoxybenzoin as a starting material and proceeded through 7 steps which contain formation of isoxazolyl ring. Result: The selective COX-II inhibitor was labeled with 18F via nucleophilic substitution reaction on the corresponding bromo or tosyl precursor in high yield. Conclusion: The selective COX-II inhibitor was labeled with 18F in high yield. We expect that these result are sufficient for animal and human studies. In this study, we will also prepare other COX-II inhibitors which are labeled with iodine, bromine and so on. And the results for biological studies will be discussed. 213 Study of the estrogen receptor binding F-18 labeled 16α[18F]fluoroestradiol K.C. Lee, B.S. Moon, K.S. Chun, C.W. Choi Korea Institute Radiological & Medical Sciences, Cyclotron Application Lab., Seoul, Korea Purpose: Estradiol is one of estrogen and produced women's ovary also it was high distribution of the uterus and the ovary. In case of manifestation of the estrogen receptor on the breast cancer, treated using by the hormone cure. Developed various estradiol derivatives and reported the radioisotopes such as I-123, Tc-99m and F-18 labeled compounds for diagnosis of the breast cancer. In this study, we want to make a diagnosis of the breast cancer and manifest of the estrogen receptor using F-18 introduced estradiol derivative. Method: We used labeling reaction precursor, 3- position protected with MOM and 16β 17β-OH groups introduced cyclic sulfone group of estradiol compound then labeled with F-18 for 10 min at 115°C. Finally, the hydrolysis step was added 3 drops of c-H2SO4, one-pot reaction. Result: The radiochemical purity was more than 95% and we separated the 16α-[18F]fluoroestradiol at 13-14 min using reverse phase HPLC system (C18 Econosil, 10 µ 50% Ethanol/H2O, flow rate: 4 mL/1 min). Total reaction time was 70 min and the radiochemical yield was more than 60%. Conclusion: The F-18 labeled estradiol is making a comparative study of ER+/ER- cell line test and obtaining the image of using micro PET then will use of the breast cancer diagnosis. Posters (T6) 214 Education, research and science promotion in stable isotope techniques M. Zubillaga, A. Barrado, C. Goldman, H. Torti, M. Martinez Sarrasague, M.Janjetic, M. Salgueiro, J. Boccio Physics Department, School of Pharmacy and Biochemistry, UBA, Buenos Aires, Argentina Stable isotope techniques are widely spread all over the world. Sometimes, this kind of technology is not routinely used in developing countries, due to the low availability of resources to support a high cost of isotopes and equipments. Even though, the School of Pharmacy and Biochemistry of the University of Buenos Aires gives the first steps in the use of stable isotopes in Physics, a subject in the second year of the Pharmacy and Biochemistry career. A thousand of students pass by their classrooms and laboratories annually. In November 2002, the Laboratory of Stable Isotopes Applied to Biology and Medicine was created with the collaboration of the International Atomic Energy Agency (IAEA). A GC-IRMS was set up through an International Project (ARCAL LIV). This new laboratory has made possible the development of research projects linked with the infection by Helicobacter pylori and other pathologies and increased the capabilities for education. It has strengthened the development of different post-degree education activities. In the same way these new facilities have also increased the international interchange of different fellows strengthened the skills of several professionals from different

developing countries. The promotion of this new isotopic methodology for our region has been our first challenge, by the performance of regional courses and the motivation of different professionals from the health sector in the routinely use of these techniques through the Science and Technology Secretary of the School of Pharmacy and Biochemistry. The aim of our work is to present the goals of this new laboratory in research, education and training of undergraduate and postgraduate students in Latin America.

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Authors not attending 215 Applications of isotopes for societal benefit in India S.M. Rao Navi Mumbai, India Thanks to an early realization of the importance of the radioisotopes in societal development, the isotope programme in India has had a substantial impact on the healthcare, industry, water resources development and agricultural productivity in India. The programme has been mainly nurtured at the Bhabha Atomic Research Centre (BARC) and the Board of radiation and isotope Technology (BRIT). It involved reactor production of over 100 radioisotopes, their processing into various physical and chemical formulations for diverse applications, development of applications in healthcare, industrial processing & quality control, nuclear agriculture and in water resources development and management. The status of the programme in India is as follows: - Nearly 150 hospitals practise nuclear medicine largely with radiopharmaceuticals supplied by BRIT - About 500 radioimmuniassay (RIA) laboratories exclusively managed by BARC - trained personnel - Nearly one million patient investigations are carried out per year using nuclear medicine procedures by doctors qualified through the Diploma in Radiation Medicine (DRM) course offered by BARC under the University of Mumbai - There are 150 teletherapy units in India using cobalt-60 sources supplied by BRIT. Here again, BARC offers a Diploma in Radiation Physics (DRP) course under the University of Mumbai to provide qualified medical physicists to teletherapy and brachytherapy centers. - India has over 30 years of experience in radiation sterilization of medical products. There are three plants in India; one each in Mumbai, Bangalore and Delhi. A fourth one in Jodhpur is a multi-purpose irradiator including for radiation sterilization. - In the field of tracer technology in industry, BARC in collaboration with the Institute of Chemical Technology of University of Mumbai, Engineers India Limited (EIL) and others has established leadership in Asia and the pacific Region. Nearly 350 major isotope tracer and sealed sources investigations have so far been carried out in Indian industry with large economic benefits. - Major steel plants and oil companies have in-house facilities for radiotracer applications. - In oil field operations, radiotracers are routinely used to look for undesirable channels in cementing behind casings, to obtain water injectivity profiles in injection wells for secondary recovery operations and to decipher the flow pattern of injection water between injection and production wells. - Isotope hydrology has come to be recognized as an integral part of water resources development and management practice in India. Besides BARC, there are seven more institutions engaged in the use of isotope techniques in hydrology. This is one area where extensive use of environmental radioisotopes and stable isotopes has been achieved for societal benefit. - Isotope tracers are today making significant contribution in investigations on transport of pollutants in surface waters including coastal seas to enable optimum design of disposal systems. - Isotope radiography for industrial NDT was one of the earliest applications of radioisotopes. Today, it is still a vibrant activity with 350 organizations offering commercial service out of the 500 organizations/industrial plants practising the technique. As part of the promotional programme, nearly 6000 persons have been trained at different levels of radiography practice - Gamma scanning for 'on line' troubleshooting in industrial systems, particularly in petrochemical complexes is well established - In the area of agriculture, radiation mutation for crop improvement has been the main use of radioisotopes. The agricultural laboratories in the country including BARC have so far released nearly 80 mutants of various crops through the radiation path. Of these, 22 have been released by BARC. These include groundnuts, mustard, rice, jute, black gram, green gram and pigeon pea.

- Isotope tracers, both radioactive and stable, have been extensively used in India for studies on soil fertility and plant nutrition. - Extensive investigations on radiation preservation of food including wholesomeness of irradiated food resulted in the Government approving the procedure for potatoes, onions, spices, wheat and wheat products, meat etc. As a result of this, the country's first spice irradiation plant is being operated in Navi Mumbai and a demonstration plant for sprout inhibition in onions is built near Nasik in Maharashtra. 216 Comparative analysis of positron spectra compression by wavelet transform and SVM approach S. Avdic Universityo f Tuzla, Faculty of Science, Department of Physics, Tuzla, Bosia and Herzegovina Positron annihilation lifetime spectroscopy (PALS) is an effective tool in defect characterization of nuclear reactor materials. If there is an open-volume defect in material, the reduction of the positron-nuclei repulsion may trap the positron at the defect. The positron in condensed matter annihilates with an electron with the emission of two back-to-back gamma photons. These gamma rays carry the information on positron lifetime and the momentum of the annihilating electron-positron pair. Defect spectroscopy is based on the fact that the annihilation parameters are changed when the positron is trapped in the defect. Lifetime of the positron trapped by the defect increases due to the reduced electron density. The main goal of PALS is to decompose the measured positron lifetime spectrum in order to find the various defect lifetimes. There are some numerical codes based on different kinds of minimization that are used for extraction of spectral parameters such as the lifetime and the intensity values of each exponential components in the measured spectrum. A new method for unfolding of positron lifetime spectra based on the use of artificial neural networks (ANNs) was suggested and tested on simulated data recently. The applicability of the method to the analysis of experimental positron spectra has been verified in the case of spectra from polymer materials. However, it has been also demonstrated that the backpropagation network has not been suitable for the identification of both the spectral parameters and the number of spectral components with a high accuracy. In general, the precision can be improved by further refining the training parameter mesh and increasing the number of iterations in the training process that would lead to much longer training times. One way to shorten training times is to perform a reduction of the training data with minimal loss of information. Support vector machine (SVM) and wavelet decomposition has been tested in order to achieve a substantial compression of input data in the ANN unfolding of positron lifetime data. It has been demonstrated that the application of wavelet transform to the positron lifetime spectra leads to a significant reduction of spectral data. It has been also shown that the SVM for regression can be successfully applied to positron spectra in achieving substantial data compression. Effectiveness of both approaches in compression of positron spectral data has not been explored yet. 217 Synthesis of multiple stabel isotope labeled R-3-aminoquinu-clidine Z. Jian, W.T. Stolle Pfizer, Inc., Isotope Chemistry, Kalamazoo, USA Many CNS agents containing the (R)-3-aminoquinuclidine moiety selectively activate the a-7 neuronal nicotinic acetylcholine receptor and are being investigated for the treatment of cognitive deficits associated with schizophrenia and Alzheimer's disease1. Current research in the area has generated the need for multiply stable isotope labeled (R)-3-aminoquinuclidine (8) as a precursor for the preparation analytical internal standards for a series of potent drug candidates. This key intermediate whose synthesis is detailed, was obtained starting from d4-isonicotinic acid (1). The chiral center was introduced by the condensation of deuterium labeled 3-quinuclidinone (5) with (S)-1-phenethylamine, followed by the reduction of the newly formed carbon nitrogen double bond.

64 April 25 – 29, 2005 5ICI

Catalytic debenzylation of (7) furnished optically pure deuterium labeled (8) in an overall 17.7% yield, compared to a 6.4% overall yield for a published C-14 synthesis through a different route2. The enantiomeric purity of (R)-3-[2H11]aminoquinuclidine was determined to be greater than 99% when converted to the final compound of interest when analyzed by chiral HPLC. 1. a) Preparation of N-(azabicyclyl)arylamides for therapeutic use as nicotinic acetylcholine receptor agonists. Jacobsen EJ, Walker DP, Wishka DG, Reitz SC, Piotrowiski DW, Acker BA, Groppi VE Jr. WO 2003072578, September 4, 2003. b) Preparation of N-(azabicyclyl)arylamides for therapeutic use as nicotinic acetylcholine receptor agonists. Rogers BN, Piotrowski DW, Walker DP, Jacobsen EJ, Acker BA, Wishka DG, Groppy VE Jr. WO 2003070732, August 28, 2003. c) Walker DP, Piotrowski, DW, Jacobsen EJ, Acker BA, Groppi VE Jr. 2003070731, August 28, 2003. 2. Synthesis of (R) and (S) 3-Aminoquinuclidine-[3-14C] Enantiomers, Important Components of a Variety of 5-HT3 Ligands. Parness H and Shelton EJ, J. Labeled Compds. Radiopharm., 1996, XXXVIII, 19-29. 218 oral Radioactive inventory estimation at the Los Alamos Isotope Production Facility using MCNPX/CINDER90 modelling M. Fassbender, F.M. Nortier, R. Heaton, H. Trellue, D.R. Phillips Los Alamos National Laboratory, Los Alamos, USA The Isotope Production Facility (IPF) is a new beam line tunnel taking off from the main beam-line of the 800 MeV Linear Proton Accelerator (LANSCE) at the transition region between the 100 MeV drift tube linac and the 800 MeV side-coupled cavity linac. IPF delivers 100 MeV protons of 250 A average beam current to a target box for radioisotope production. The authorization basis allows the facility to be operated as a low hazard, radiological facility per definitions and guidance given in DOE Standard 1027-92 to facilitate compliance with DOE Order 5480.23. The hazard categorization of the facility requires that total radionuclide inventories in the facility never exceed the Category 3 Nuclear Facility threshold. In order to estimate activity amounts of radioisotopes produced at IPF prior to production runs, the Monte Carlo code MCNPX in combination with the code CINDER90 has been used. MCNPX has also been employed to simulate proton and neutron fluence profiles for the IPF facility. This paper presents computed radionuclide activity estimates as compared to experimental yields obtained via chemical processing of irradiated target materials. Furthermore, simulated neutron and proton fluence distributions for IPF are introduced. Target materials included stainless steel, Al, Inconel, RbCl, Nb, and Ga. It was observed that MCNPX/CINDER90 generally overestimated the actual amount of radioactivity produced at IPF in target materials containing by a factor of 2-3.

5ICI April 25 – 29, 2005 65 Author Index

Aaltonen, J. 133 Abbas, K. 6 Abdel-Halim, A. 191 Adam-Rebeles, R. 170 Adamenko, A.S. 50 Adamenko, S.V. 50 Afarideh, H. 158 Ahn, G.I. 11 Akhlaghi, M. 189 Alami, R. 93 Alanis, J. 145 Alanis-Morales, J. 142 Albert, P. 73 Alekseev, I.E. 16, 29, 30 Allen, B. 2 Altieri, S. 118 Altzitzoglou, T. 57, 79 Amaral, P. 190 An, G. 212 An, J. 92 Andreotti, E. 86 Andres, H. 64 Andreyev, O.I. 24, 27, 34, 35 Apostolidis, C. 120, 122, 123a Aravena, R. 5, 192 Arjun, G. 152 Arlinghaus, H. 115 Asadollahi, Z. 164 Aslani, G. 33, 126, 141, 155, 157 Avdic, S. 216 Baba, M. 173, 176 Babaie, H. 100 Babaii, M. 189 Baccus, M. 49 Bakhtiari, H. 71, 164 Bakker, C.J. 204 Ball, G. 15 Baranov, A.Y. 27 Baranov, V.Y. 45, 148 Baranyai, L. 143 Baro, G. 109 Barrado, A. 214 Basilico, F. 114 Beets, A.L. 38 Bekker, A.J. 134 Benahmed, A. 93 Bendassolli, J.A. 5, 190, 192 Bensimon, C. 69 Benzhu, C. 25 Bergoc, R. 135 Berthelette, C. 65 Betak, E. 174 Beyer, G. 119 Bianchin, A. 135 Bickel, M. 79 Bigelow, T.S. 41, 165 Bin, X. 102 Birattari, C. 128 Birebent, G. 123 Bizet, P. 23 Blust, R. 22 Boccio, J.R. 201, 214 Bodart, F. 39 Boeyens, J.C.A. 52 Bogod, V.B. 150 Bohnstedt, A. 79 Bokhan, P.A. 43, 56 Bonardi, M.L. 128 Bonet, H. 9 Borisevich, V.D. 46

Bortolussi, S. 118 Braghieri, A. 118 Brans, B. 8 Brawner, J. 32 Broelsch, C. 117 Brown, D.J. 32 Brown, R.W. 144 Bruchertseifer, F. 123a Bruschi, P. 118 Bubas, O.V. 151 Butler, M.J. 76 Bychkov, A. 47 Calmanovici, G.P. 135, 201 Canella, L. 128 Capote, R. 174 Carlson, B.V. 174 Cha, Y.H. 20 Chaidhri, M.N. 121 Chan, A. 69 Chang, H.-H. 95, 194 Chang, K. 131 Charif, A. 93 Charlton, J.S. 4 Chattopadhyay, S. 152, 160, 161 Chaudhri, M.A. 55, 82, 101 110, 121 Chaudhri, M.N. 55, 82, 110 Cheltsov, A.N. 150 Chen, B. 210 Chen, D. 98 Cherednichenko, S.A. 46 Cherkaoui, R. 93 Chiper, D. 73 Cho, K. 131 Cho, S.H. 17 Cho, W.K. 132 Choi, C.W. 11, 212, 213 Choi, H.-D. 174, 177 Choi, H.S. 19 Choi, O. 19 Choi, S.M. 153, 202 Choung, W.M. 153 Chudakov, V. 31 Chun, K.S. 11, 212, 213 Chung, H.-Y. 95, 194 Chung, J.K. 104 Chuvilin, D.Y. 144, 208 Cocca, C. 135 Coenen, H.H. 53 Cohen, D. 1 Colli, V. 113 Cong, P. 92 Courtney, W. 32 Cozar, O. 170 Cremaschi, G. 135 Cricco, G. 135 Csikai, J. 173, 176 Cui, H. 98 Daming, C. 25 Dana, A. 15 Danaila, L. 187 Danks, P. 69 Daraban, L. 170, 170, 172 Darbyshire, J. 66 Darmograi, V.V. 29 Das, M.K. 103, 149, 152,160, 161 David, B. 9, 23, 138 Davio, C. 135 De Boeck, G. 22 De la Paz-Luna, M. 97, 206

De Lellis, C. 84 De Meyer, M. 106, 178 de Roos, R. 204 De Smedt, F. 23 De Vos, F. 138 Debauche, A. 84 Decaillon, J.G. 79 Deleanu, C. 183 Diaz, M.E. 97, 206 Diaz-Bustos, E. 206 Ding, W. 130 Ding, Y. 111 Ditroi, F. 173, 176 Domanov, V.P. 40, 81 Dong, W.J. 111 Du, J. 98 Du, M. 38 Dvoretsky, V.V. 169 Dyatlov, A.A. 44 Ebadati, J. 54 Efimov, V.N. 169 El Badri, L. 93 El-Taher, A. 191 Elwan K.M. 96 Emery, M. 66 Encut, I. 184 Ensaf, M. 211 Erilov, P. 31 Ervanne, H. 133 Eursch, A. 123 Fan, X. 88 Fassbender, M. 218 Fateev, N.V. 43, 56 Fateh, B. 155 Fei, T.X. 111 Fekry, A.E. 96 Ferrari, C. 114, 118 Ferrer, L. 129 Fiederer, K. 28 Filimonov, V.T. 35 Fink, D. 1 Fossati, F. 118 Fretz, M.M. 112 Fu, Z.L. 124 Fugaru, V. 182, 183, 184, 198 Fujiyoshi, R. 74 Fülöp, F. 67 Galico-Cohen, L. 142 Gambarini, G. 113 Garland, M. 38 Gasparro, J. 80 Gavrilov, V.D. 24, 34, 35 Gay, S. 113 Genaro, A. 135 Gerardy, I. 89 Gerstenberg, H. 28 Gevorkyan, M. 200 Geza, T. 67 Ghasemi, M. 164 Ghazlane, H. 93 Gibson, N. 6 Gilles, C. 138 Giuliani, A. 86 Gnidoi, I.P. 44 Goede, A. 51 Goetz, C. 117 Goldberg, M. 37 Goldman, C.G. 135, 214, 201 Goldman, S. 127 Gonzalez-Calderin, S. 97, 206

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Good, S. 69 Gouveia, S.E.M. 5, 190, 192 Goverdovski, A.A. 48 Grabbe, S. 117 Grigoriev, G.Y. 44, 45, 163 Gromova, E.A. 133 Groppi, F. 128 Gu, J. 105 Guérit, N. 106 Guillaume, J. 89 Guo, F.Q. 107, 124 Guo, X. 91 Guo, Z. 130, 210 Gusev, V.V. 148 Gutierrez, A. 135 Gutierrez, H. 109 Gwan, H.J. 202 Gwon, H.J. 186 Haas, R. 120, 122 Haddad, F. 129 Hagiwara, M. 173, 176 Haji-Saeid, M. 10 Hajilo, N. 157 Hamidi, S. 157 Han, H.S. 14, 19, 146, 147 Han, J.M. 20 Hantson, A. 106, 178 Harfensteller, M. 123 Harms, A.V. 22 Hartmann, W. 21 Haselsberger, K. 117 Hassan, H.E. 53 Hattink, J. 22 Hayashi, A. 181 He, Y.J. 70 Heaton, R. 218 Heimans, J. 117 Helariutta, K. 133 Henderson-Sellers, A. 1 Henkelmann, R. 123 Hermanne, A. 37, 176 Hernandez-Triana, M. 97, 206 Hickman, D. 66 Hideghety, K. 117 Hill, C. 79 Holden, P. 1 Hollinger, R. 21 Hollins, S. 1 Holmes, L. 79 Holzwarth, U. 6 Hong, S. 147 Hong, Z. 102 Honwei, Y. 25 Host, V. 49 Hubert, R. 39 Huebner, A. 21 Huenges, E. 123 Huiskamp, R. 115 Hult, M. 80 Hupf, H. 32 Hwaree, A. 99 Ilyin E.K. 208 Ingram, A. 88 Ionita, G. 199 Jabbar, Q. 55, 121 Jacobsen, G. 1 Jakovlev, V.A. 30, 133 Jalali, M. 54, 77, 171, 175 Jalilian, A.R. 71, 126, 159, 189 211

Jang, S.H. 186 Jang, Y.-S. 95, 194 Jansen, D. 18 Jeon, I.Y. 132 Jeon, K.H. 132 Jeong, D.Y. 20 Jeong, J.M. 104 Jia, B. 98 Jian, Z. 217 Jin, G. 102 Jin, X. 98 Jiskoot, W. 112 Johari Daha, F. 62, 179 Jokela, T. 188 Jun, B.J. 146 Kabai, E. 123 Kadiata, M. 127 Kaizer, G. 115 Kajiwara, M. 181 Kamali Moghadam, K. 141 Kamali-Dehghan, M. 71, 126,159 189 Kamanin, D. 48 Kang, P.H. 94, 196, 197 Kang, P.K. 195 Kanygin, V. 200 Karmann, I. 190 Keck, B. 60 Keightley, J. 57 Kemmler, W. 101 Keresztes, A. 67 Khadra, M. 185 Khairy, M.A. 191 Khan, M.A.S. 90 Khoroshilov, A.V. 46 Khvostionov, V.E. 144 Kiefer, J. 109 Kim, B. 125 Kim, C. 125 Kim, C.J. 20 Kim, C.S. 177 Kim, E. 125 Kim, H.I. 146 Kim, I.S. 17 Kim, J. 11, 177 Kim, K.H. 132 Kim, M.J. 202 Kim, M.S. 153 Kim, S. 205 Kim, S.J. 153, 202 Kim, S.K. 20 Kim, S.S. 195 Kim, Y.J. 104, 132 Kim, Y.N. 104 Kindler, B. 21 Király, B. 176 Kisly, V.A. 169 Klecha, A. 135 Klein, J.A. 38 Klimov, S.I. 25, 151 Kliszewski, S. 120 Knapp, F.F. 38 Knoesen, O. 72 Kolar, Z.I. 18, 137 Koning, G.A. 112, 204 Konya, J. 143 Kormilitsyn, M.V. 47 Kornilov, A.S. 35 Kornilova, A.A. 168 Korsak, A. 68

Kostenikov, N. 31 Koulmanda, M. 110 Kovalev, S.F. 173, 176 Kozar, A.A. 167 Krasnov, N.N. 156 Krijger, G.C. 18, 22, 112, 204 Kronenwett, R. 120, 122 Krukov, F.N. 169 Kudelin, B. 154 Kuo, F. 59 Kupriyanov, V.N. 34, 35 Kupsch, H. 78 Kuznetsov, R.A. 25, 35, 151 Kwon, D.H. 20 Lacroix, J.-P. 84 Lambert, B. 138 Laraki, K. 93 Lavie, E. 37 Lazarev, V.V. 16, 30 Lebedeva, L.S. 5, 85, 167 Ledru, M.P. 5 Lee, B.H. 132 Lee, B.I. 177 Lee, C.S. 177 Lee, D.H. 11 Lee, D.S. 104 Lee, H.Y. 104 Lee, J.K. 177 Lee, J.S. 11, 14, 19, 146 Lee, K. 125 Lee, K.C. 213 Lee, M. 181 Lee, M.C. 3, 104 Lee, S.M. 197 Lee, Y.-K. 95, 194 Lee, Y.J. 104 Leonardi, N.M. 201 Leonov, A.I. 156 Leppälä, E. 61 Letsoalo, M. 72 Li, C. 65 Li, X. 28 Li, Z. 105 Lidia, M. 184 Lim, Y.K. 177 Liu, B. 130 Liu, J. 92 Liu, X.Y. 70 Lommel, B. 21 Loquai, C. 115 Lucas, S. 39, 108 Lunden, A. 133 Lungu, V. 73, 187 Luo, S.N. 70 Luo, Z. 98 Lützenkirchen, K. 83 M. Nagy, N. 143 Ma, D. 98 Maecke, H.R. 69 Makkonen-Craig, A. 133 Malyugin, S.L. 163 Mangood, S.M. 96 Mansel, A. 78 Markovskij, D.V. 144, 208 Martin, G. 135 Martin, S. 120, 122 Martinez Sarrasague, M. 214 Martinotti, A. 128 Matei, L. 182, 183, 198 Matloubi, H. 62, 63, 179, 180

5ICI April 25 – 29, 2005 67 Author Index

Matthies, A. 48 Mauri, P. 114 Mayer, K. 83 Mayorshin, A.A. 47, 169 McCracken, N. 66 Medina, J. 32 Medina, V. 135 Melnichenko, N. 200 Menapace, E. 128, 174 Meyer, W. 166 Michel, J. 115 Mikolajczak, R. 36, 68 Millet, S. 83 Mimount, S. 93 Mirzadeh, S. 38 Mirzaii, M. 71, 126, 155, 159 189 Mitchell, P. 139 Moafian, J. 71, 189 Mohamed, N. 135 Mohati, M. 164 Molinet, R. 122, 123a Monclus, M. 127 Monn, J. 58 Monroy-Guzman, F. 142 Moon 193 Moon, B.S. 213 Moradkhani, S. 189 Moreno Bermudez, J. 123 Morgenstern, A. 120, 122, 123a Morzenti, S. 128 Moss, R.L. 112, 115, 116, 117 Mostaan, M. 189 Mostajab Davati, M. 54, 77 Mukherjee, A. 103 Mulleneers, E. 127 Müller, H.W. 122 Myasoedov, N.F. 66 Nabiev, S. 163 Nadeem, Q. 55, 121 Nadezhdinskiy, A.I. 163 Nagaev, I.Y. 66 Nair, K.V.V. 103 Najafi, R. 100 Nam, S.M. 20, 147 Nano, R. 118 Navarrete, J.M. 145 Negoita, N. 183, 198 Nerozin, N. 200 Neumann, F. 122 Nho, Y.C. 94, 195, 196, 197 Nicolini, J. 109, 203 Nicolini, M. 203 Niculae, D. 73, 187 Niels, Y. 49 Niemann, D.J. 72 Nievaart, S. 116 Nievaart, V.A. 112 Nijsen, J.F.W. 204 Nikitina, E.A. 42 Noorkojoori, H. 71 Nortier, F.M. 174, 218 Novinrooz, A.J. 164 Novoselov, A.E. 169 Nunez, M. 135 Nuttens, V. 108 O'Bannon D. 58 Odintsov, A. 168 Oelsner, S. 69 Offner, F. 120

Oh, S.Y. 17 Okhotina, I.A. 42 Olsen, S.C. 140 Omidvar, M. 54 Orion, I. 99 Oyen, W. 8 Paces, T. 74 Paeng, J.Y. 202, 205 Pagano, T. 66 Pakhomov, A.N. 25, 151 Pal, S. 103, 160, 161 Panait, M. 184 Paquis, P. 117 Park, H. 11, 20 Park, J. 147, 193 Park, J.H. 153 Park, K.B. 14, 17, 19, 153, 186 205 Park, K.R. 94 Park, S.H. 153, 186, 202 Park, U. 146, 147 Park, U.J. 14, 19 Parker, D. 88 Parus, J.L. 36, 68 Pasini, E. 207 Paviotti de Corcueara, R. 174 Pavlikhin, V.E. 156 Pavlovich, V.N. 168 Pavshook, V.A. 144 Pawlak, D. 36, 68 Payne, T.E. 1 Pedretti, M. 86 Pedroni, P. 118 Pellicciari, M. 86 Perera, O. 185 Peretroukhin, V.F. 167 Perhola, O. 133 Peshkov, A.T. 44 Pessenda, L.C.R. 5, 190, 192 Peterson, E. 31 Petrovich, C. 113 Phetoe, M.M. 139 Phillips, D. 31 Phillips, D.R. 218 Pietzch, H.-J. 186 Pinelli, T. 118 Podina, C. 182 Podsoblyaev, D. 200 Pohjoispää, M. 61 Pommé, S. 57 Ponsard, B. 22, 26 Ponurovskiy, Y. 163 Pooladi, M. 189 Popescu, I. 199 Postolache, C. 182, 183, 184, 198 Prinsloo, R.H. 15 Purice, M. 187 Pustovalov, A.A. 148 Qaim, S.M. 53, 174 Qi, B. 98 Radchenko, V.M. 85, 167 Rahiminejad, A. 33 Rahnama, M. 100 Raisali, G. 13, 126, 157 Rajabi, H. 100 Ramamoorthy, N. 10, 149, 152 Rao, S.M. 215 Rasaee, M. 100 Raspopov, A. 200 Raty, P. 49

Rav, H.L. 7 Razbash, A. 156 Revyakin, Y.L. 35 Rezaee, K.H. 77 Rhee, Y. 20 Ribeiro, A.S.R. 5, 192 Rivera, E. 135 Rocher, L. 89 Rogov, A.D. 48 Romanov, E.G. 167 Romanow, A. 123a Rosi, G. 113 Rotert, G. 66 Rotmanov, K.V. 167 Rowshanfarzad, P. 71, 126, 159 189, 211 Ruiz-Alvarez, V. 97, 206 Ryabinin, M.A. 85 Ryzhkova, D. 31 Sabet, M. 126, 159, 211 Saddadi, F. 189 Sadeghi, M. 71, 158 Sadri, H. 164 Saemian, N. 62, 63, 179, 180 Saia, S.E.M.G. 190, 192 Sakamoto, K. 74 Salazar, G. 206 Salazar-Rodriguez, G. 97 Salvatores, M. 57a Sanchez-Alvarez, G. 97 Saraswathy, P. 152 Sarkar, S.K. 152 Sarma, H.D. 103 Sasinowska, I. 68 Sattari, A. 33, 141 Sauerwein, W. 114, 115, 116 117, 207 Sawamura, S. 74 Scheigetz, J. 65 Schilp, M. 123 Schmidt, D. 122 Schmitz, F. 127 Scholten, B. 53, 174 Seals, J. 32 Seifert, B. 186 Seifu, K. 75 Selome, J. 134 Semenov, A.O. 34 Seong-Ae 193 Seppenwoolde, J.H. 204 Serban, V. 183 Sevastianov, Y.G. 156 Seyedi, H. 164 Shababi, I. 54 Shadanpour, N. 33, 141 Shady, S.A. 51 Shafaii, K. 189 Shahabi, I. 54 Shani, G. 99 Shapovalov, B. 200 Shen, J. 107 Shevchenko, V.P. 66 Shibata, M. 74 Shin, B. 153, 202 Shin, B.C. 205 Shin, H.S. 17 Shin, Y.J. 17 Shirazi, B. 155, 158 Shirvani, G. 62, 63, 179, 180 Shishalov, O.V. 47, 169

68 5ICI

Shrivastava, S. 24 Shubin, A.N. 42 Shubin, Y.N. 173, 174, 176 Sibbens, G. 57, 79 Sifeddine, A. 5, 190 Skiba, O.V. 47 Skorynin, G.M. 42 Slegers, G. 138 Smetanin, E. 200 Smith, M.D. 88 Smith, M.E. 134 Soberano, M. 203 Solin, L.M. 30, 154 Son, K.J. 14, 146, 147 Son, M. 104 Sosnin, L.Y. 150 Spellerberg, S. 53 Spence, M. 59 Stamm, H. 6 Stavrovskiy, D.B. 163 Stecher-Rasmussen, F. 116, 117 Stefanescu, I. 199 Steiner, J. 21 Stevenson, N.R. 41, 165 Stolle, W.T. 217 Storm, G. 112 Stratton, T. 66 Sublet, J.-C. 174 Sudersanan, M. 161 Sumiyoshi, T. 74 Surber, B. 66 Surdersanan, M. 160 Susan, A.B. 66 Suzuki, M. 74 Suzuki, Y. 74 Swanson, S. 66 Szántó, Z. 57 Szemenyei, E. 67 Takacs, S. 37, 176 Takatori, K. 181 Tamiru, A. 75 Tarallo, F.J. 41, 165 Tarasov, V.A. 27, 34, 35, 151 167 Tarkanyi, F. 174, 176 Tarkanyi, J.-F. 173 Tashirev, A.B. 168 Tenalem, A. 75 Teykovtsev, A.A. 169 Therasse, P. 115, 117 Thierens, H. 138 Thome, L. 144 Tian, H. 124 Tian, J. 210 Tian, J.H. 130 Tikhomirov, A.V. 148, 162 Tinschert, K. 21 Tkharkakhova, S.R. 16 Tondeur, F. 89 Toporov, Y.G. 24, 34, 35, 167 Trellue, H. 218 Tsvetkov, L.A. 148 Tuovinen, H. 133 Türler, A. 123 Tyutin, L. 31 Uddin, M.S. 173, 176 Udovenko, A.N. 144 Ughetti, R. 109, 203 Ustinov, A.L. 44, 163 Vakhetov, F.Z. 24, 35

Valente, M. 113 Valli, M. 58 Van Ammel, R. 57 Van den Winkel, P. 172 Van Gansbeke, B. 127 van het Schip, A.D. 204 van Loenen, A. 117 Van Loon, R. 136 Van Naemen, J. 127 Van Put, P. 84 Van Tiggelen, R. 136 van Wyk, E. 76 Vandenbulcke, K. 120 Varlam, C. 199 Vedoveto, M. 192 Venkatesh, M. 149 Vente, M.A.D. 204 Verhagen, B. 76 Vimalnath, K.V. 149 Vincent, J. 31 Vysotskii, V.I. 50, 168 Wagener, J.M. 185 Wähälä, K. 61, 188 Wallenius, M. 83 Wang, F. 98 Wang, H.Y. 70 Wang, L. 92 Wang, R.F. 107, 124 Wang, Y.F. 124 Wätjen, U. 57, 80 Watling, J. 101 Wheeler, W. 58, 59 Williams, A. 1 Wittig, A. 114, 115, 116, 117 207 Woroniecka, U.D. 112 Wu, H. 92 Wu, Z. 91 Xie, M.H. 70 Xu, B. 105 Yan, F. 124 Yan, H. 102 Yan, Z. 102 Yang, H. 98 Yang, X.F. 124 Yang, Z. 105 Yao, S. 130 Yin, D. 130 Zakrevsky, D.E. 43, 56 Zamboni, R. 65 Zeevaart, J.R. 18, 51, 139 Zhang, C.L. 107, 124 Zhang, H. 105 Zhang, J. 12, 98, 130, 210 Zhang, X.C. 124 Zhao, G.Y. 124 Zhao, P. 87 Zhemkov, I.Y. 47, 169 Zhenfu, L. 102 Zhi, Y. 102 Zhuikov, B. 31 Zhukovsky, E.A. 150 Zielhuis, S.W. 204 Zierold, K. 115 Zimmermann, R. 74 Zona, C. 128 Zonneberg, B.A. 204 Zonta, A. 114, 118 Zotov, E.A. 27, 34 Zubillaga, M. 135, 201, 203, 214