International Journal of Civil, Structural,

Environmental and Infrastructure Engineering

Research and Development (IJCSEIERD)

ISSN 2249-6866

Vol. 3, Issue 4, Oct 2013, 17-26

© TJPRC Pvt. Ltd.

CADMIUM REMOVAL FROM AQUEOUS SOLUTION BY MODIFIED LOW COST

ADSORBENT(S): A STATE OF THE ART

NITIN W. INGOLE1 & VIDYA N. PATIL

2

1Professor and Head, Department of Civil Engineering, Prof Ram Meghe Institute of Technology & Research, Badnera,

Amravati, Maharashtra, India

2Assistant Professor, Department of Civil Engineering, All India Shri Shivaji Memorial Society’s College of Engineering,

Pune, Maharashtra, India

ABSTRACT

The agricultural waste has been investigated as a replacement for costly methods of removing heavy metal from

water. Cadmium (Cd) is one of the heavy metals, which is highly toxic to human, plants and animals. Some of agricultural

waste can be effectively used as a low cost adsorbent in cadmium adsorption. Modification could enhance their natural

capacity and add value to the adsorbent. In general, chemically modified plant wastes exhibit higher adsorption capacities

than unmodified forms. Numerous chemicals have been used for modifications which include mineral and organic acids,

bases, oxidizing agent, organic compounds, etc. In this review, Agricultural wastes as adsorbents including Rice husk,

Sawdust (cedrus deodhar wood), Sawdust (Pinus sylvestris), Walnut sawdust, Juniper fibre, Sugarcane bagasse, Wheat

bran, Cassava, tuber bark waste, Cassava waste, Corncorb, Coirpith, and others has been compiled. Some of the modified

adsorbents show good adsorption capacities for Cd, The present paper reviews various techniques being followed and

research efforts being made for removal of Cd(II) from aqueous solutions with modified adsorbents.

KEYWORDS: Cadmium, Adsorption, Agricultural Waste Adsorbents, Modified Adsorbents

INTRODUCTION

Water pollution due to toxic heavy metals has been a major problem. As a consequence, cadmium (Cd) is

produced mainly as a byproduct from mining, smelting, and refining of sulfide ores of zinc. The metal is of special concern

because it is non-degradable and therefore persistent. The task of providing proper treatment facility for all polluting

sources is difficult and also expensive, hence there is pressing demand for innovative technologies which are low cost,

require low maintenance and are energy efficient (Renge et al., 2012).

Research interest into the production of cheaper adsorbents to replace costly water treatment methods such as

chemical precipitation, ion exchange, electro flotation, membrane separation, reverse osmosis, electro dialysis, solvent

extraction etc is there. The adsorption technique is economically favorable and technically easy to separate as the

requirement of the control system is less (Zacaria R 2002, Acar, F.N. and Eren, Z., 2006, Amit et al., 2010). Researchers

have worked on inexpensive materials, such as Rice husk, Sugarcane bagasse, Wheat bran, tuber bark waste, Corncorb,

Coirpith which have Cd adsorption capacity and are locally available agricultural waste.

Some of the advantages of using plant wastes for wastewater treatment include simple technique, requires little

processing, good adsorption capacity, selective adsorption of heavy metal ions, low cost, free availability and easy

regeneration. However, the application of untreated agricultural waste adsorbents can also bring some problems such as

low adsorption capacity, high chemical oxygen demand (COD) and biological oxygen demand (BOD) as well as total

18 Nitin W. Ingole & Vidya N. Patil

organic carbon (TOC) due to release of soluble organic compounds contained in the plant materials (Gaballah et al., 1997;

Nakajima and Sakaguchi, 1990, Crini and Badot 2008). The increase of the COD, BOD and TOC can cause depletion of

oxygen content in water and can threaten the aquatic life. Therefore, agricultural wastes need to be modified or treated

before being applied for the decontamination of heavy metals (Deshkar et al., 1990, Taty et al., 2003, D. Kołodyńska

2011). In this review, list of adsorbents obtained from agricultural wastes has been compiled and their methods of

modification are discussed.

AGRICULTURAL WASTE ADSORBANTS

The surfaces of solids or liquids possess a residual field of force which gives rise to the process of uptake of

atoms, molecules, ions from the systems in contact, this phenomenon is known as ‘adsorption’. The system which retains

the foreign species at the interface is known as the adsorbent and the retained species are referred to as the adsorbate. The

adsorption is categorized on the basis of interactions involved between the atoms, molecules or ions or adsorbate and

adsorbent. Adsorption is one the physico-chemical treatment processes found to be effective in removing heavy metals

from aqueous solutions. According to (Bailey et al., 1999), an adsorbent can be considered as cheap or low-cost if it is

abundant in nature, requires little processing and is a byproduct of waste material from waste industry. Agricultural wastes

are inexpensive as they have no or very low economic value.

The rate of adsorption depends upon external mass transfer, internal diffusion and surface adsorption. Most of the

adsorption studies have been focused on unmodified plant wastes such as Black gram husk (Saeed and Iqbal., 2003),

Redwood bark (Masri et al., 1974), rice husk ash and neem bark (Kashiwa et al., 2000, Kumar and Bandyopadhyay,2006,

Bhattacharya et al., 2006), Waste tea, Turkish coffee, Walnut shell (Orhan and Buyukgungor, 1993). Some more

unmodified adsorbents like papaya wood (Saeed et al., 2005), maize leaf (Babarinde et al., 2006), teak leaf powder (King

et al., 2006), lalang (Imperata cylindrica) leaf powder (Hanafiah et al., 2007), rubber (Hevea brasiliensis), leaf powder

(Hanafiah et al., 2006a,b), red fir sawdust (Bryant PS et al., 1992), Coriandrum sativum (Karunasagar et al., 2005), peanut

hull pellets (Johnson et al., 2002), sago waste (Quek et al., 1998), saltbush (Atriplex canescens) leaves (Sawalha et al.,

2007a,b), tree fern (Ho and Wang, 2004; Ho et al., 2004; Ho, 2003), grape stalk wastes (Villaescusa et al., 2004), etc. also

are studied. The agricultural wastes and their maximum cadmium adsorption capacities are shown in Table 1.

Table 1: Unmodified Agricultural Waste Adsorbents

Sr. No. Adsorbents Q max (mg g-1

) Source

1 Modified wool 87 Masri and Friedman, 1974

2 Black gram husk 49.74 Saeed and Iqbal., 2003

3 Redwood bark 32 Randall et al., 1974

4 Black oak bark 29.9 Zacaria et al., 2002

5 Redwood bark 27.6 Masri et al., 1974

6 Black oak bark 25.9 Teles and Beca, 1994

7 Rice husk ash 20.24 Kumar and Bandyopadhyay,2006

8 Pine bark 14.16 Zacaria et al., 2002

9 Bamboo Charcoal 12.08 Fa et al., 2010

10 Rice husk 8.58 Kumar and Bandyopadhyay 2006

12 Waste tea 1.63 Orhan and Buyukgungor, 1993

CHEMICALLY MODIFIED AGRICULTURAL WASTES

Chemically modified agricultural wastes pretreatment of agricultural wastes can extract soluble organic

compounds and enhance chelating efficiency (Gaballah et al., 1997, Pejic et al., 2011, Crini 2005, Crini and Badot 2008).

Pretreatment methods using different kinds of modifying agents such as base solutions (sodium hydroxide, calcium

Cadmium Removal from Aqueous Solution by Modified Low Cost Adsorbent(s): A State of the Art 19

hydroxide, sodium carbonate) mineral and organic acid solutions (hydrochloric acid, nitric acid, sulfuric acid, tartaric acid,

citric acid, thioglycollic acid), organic compounds (ethylenediamine, formaldehyde, epichlorohydrin, methanol), oxidizing

agent (hydrogen peroxide), dye (Reactive Orange 13), etc. for the purpose of removing soluble organic compounds,

eliminating colouration of the aqueous solutions and increasing efficiency of Cd adsorption have been performed by many

researchers (Hanafiah et al., 2006a; Reddy et al., 1997; Taty-Costodes et al., 2003; Gupta et al., 2003; Namasivayam and

Kadirvelu, 1997; Min et al., 2004; Kumar and Bandyopadhyay, 2006; Baral et al., 2006; Acar and Eren, 2006; Rehman et

al., 2006; Abia et al., 2006; Shukla and Pai, 2005, Low et al., 1995; Azab and Peterson, 1989; Lazlo, 1987; Wankasi et al.,

2006). The types of some chemicals used for modifying specific agricultural wastes and their maximum adsorption

capacities are shown in Table 2.

Table 2: Modified Agricultural Waste Adsorbents

Sr.

No. Adsorbent Modifying Agent(s)

Q max

(mg g-1

) Source

1

Rice husk

Water washed 8.58

Kumar and

Bandyopadhyay (2006)

2 Epichlorohydrin 11.12

3 Sodium bicarbonate 16.18

4 Sodium hydroxide 20.24

5 Sawdust Formaldehyde in sulfuric acid 9.29 Taty-Costodes et al. 2003

6 Walnut sawdust Formaldehyde in sulfuric acid 4.51 Bulut and Tez (2003)

7 Juniper fibre Sodium hydroxide 29.54 Min et al. (2004)

8 Sugarcane

bagasse

Sodium bicarbonate 189

Junior et al., (2006) 9 Ethylenediamine 189

10 Triethylenetetramine 313

11 Wheat bran Sulfuric acid 101 O zer and Pirinc¸c¸ i (2006)

12

Corncorb

Nitric acid 19.3 Leyva-Ramos et al. (2005)

13 Citric acid 55.2

14 Sulfuric acid and ammonium persulphate NA Kadirvelu et al. (2001a)

Modification of Rice Husks Adsorbent

Rice husk consists of cellulose (32.24%), hemicelluloses (21.34%), lignin (21.44%) and mineral ash (15.05%) as

well as high percentage of silica in its mineral ash, which is approximately 96.34%. Rice husk is insoluble in water, has

good chemical stability, has high mechanical strength and possesses a granular structure, making it a good adsorbent

material for treating Cd from wastewater. Rice husk can be used to treat Cd in the form of either untreated or modified

using different methods. Hydrochloric acid (Kumar and Bandyopadhyay, 2006), sodium hydroxide (NAOH) (Guo et al.,

2003; Kumar and Bandyopadhyay, 2006), sodium carbonate (Na2CO3) (Kumar and Bandyopadhyay, 2006),

epichlorohydrin (C3H5ClO) (Kumar and Bandyopadhyay, 2006), and tartaric acid (Wong et al., 2003a; Wong et al., 2003b)

are commonly used in the chemical treatment of rice husk. Pretreatment of rice husks can remove lignin, hemicellulose,

reduce cellulose crystallinity and increase the porosity or surface area. In general, chemically modified or treated rice husk

exhibited higher Cd adsorption capacities than unmodified rice husk. For example, Kumar and Bandyopadhyay (2006)

reported that rice husk treated with sodium hydroxide, sodium carbonate and epichlorohydrin enhanced the adsorption

capacity of cadmium. The base treatment using NaOH for instance appeared to remove base soluble materials on the rice

husk surface that might interfere with its adsorption property. Tarley et al., (2004) found that adsorption of Cd increase by

almost double when rice husk was treated with NaOH.

Meanwhile, most of the acids used for treatment of agricultural wastes were in dilute form such as sulfuric acid,

hydrochloric acid and nitric acid. According to Pejic et al., (2011) , Esteghlalian et al., (1997), dilute acid retreatment using

sulfuric acid can achieve high reaction rates and improve cellulose hydrolysis. Concentrated acids are powerful agents for

20 Nitin W. Ingole & Vidya N. Patil

cellulose hydrolysis but they are toxic, corrosive and must be recovered (Kołodyńska 2011, shukla and pai 2005, Sivers

and Zacchi, 1995). However, in some cases, hydrochloric acid treated rice husk showed lower adsorption capacity of

cadmium than the untreated rice husk (Kumar and Bandyopadhyay, 2006). When rice husk is treated with hydrochloric

acid, adsorption sites on the surface of rice husk will be protonated, leaving the heavy metal ions in the aqueous phase

rather than being adsorbed on the adsorbent surface. Dyestuff treated rice husk using Procion red and Procion yellow for

the removal of Cd(II) were studied by Suemitsu et al., (1986).

Modification of Sugarcane Bagasse Adsorbent

Junior et al., (2006) reported the use of succinic anhydride modified sugarcane bagasse for treatment of Cd from

aqueous solutions. Sugarcane bagasse consists of cellulose (50%), polyoses (27%) and lignin (23%). The presence of these

three biological polymers causes sugarcane bagasse rich in hydroxyl and phenolic groups and these groups can be modified

chemically to produce adsorbent materials with new properties. It was found that sugarcane bagasse treated with ethylene

diamine and triethylene tetramine shows a remarkable increase in nitrogen content compared to untreated sample, and

triethylene tetramine modified sugarcane bagasse has a higher increasing extent.

The presence of amide group was also detected in ethylene diamine and triethylene tetramine modified sugarcane

bagasses as a result of the reaction between – carboxylic acid (COOH) and – NH2 groups. Kinetic studies showed that

equilibrium time for adsorption of Cd onto tethylene diamine and triethylene tetramine modified sugarcane bagasses were

slower than that for adsorbent modified with Sodium bicarbonate or sodium hydrogen carbonate (NaHCO3). Triethylene

tetramine modified sugarcane bagasse was the best adsorbent material for removal of Cd since the adsorption capacities for

both metals are two times higher than unmodified sugarcane bagasse. This was probably caused by the higher number of

nucleophilic sites introduced in triethylene tetramine modified sugarcane bagasse.

Modification of Sawdust

Sawdust contains various organic compounds (lignin, cellulose and hemicellulose) with polyphenolic groups that

could bind heavy metal ions through different mechanisms. A comparative study on the adsorption efficiency of untreated

and NaOH treated sawdust of cedrus deodar wood was conducted by Memon et al. (2007). They reported that cedrus

deodar sawdust mainly consists of acid detergent fibre (cellulose and lignin), hydroxyl groups (tannins) and phenolic

compounds. The acidimetric–alkalimetric titration study revealed that sawdust has four major groups responsible for

cadmium binding which were carboxylic, phosphoric, amines and phenolic.

Cadmium removal was more favored by NaOH treated sawdust as the value of adsorption capacity was four times

greater than untreated sawdust. NaOH treated sawdust also shows good settling property, making it easy to filter or

separate the adsorbent from the solution. Maximum adsorption capacity recorded at temperature of 200C was 73.62 mg g

-1.

Two kinds of sawdust, poplar and fir wood were treated with treated with NaOH (fibre-swelling agent) and Na2CO3

solutions and the adsorption capacities were compared with the untreated sawdusts (Taty-Costodes et al. 2003).

A detail analysis on the ideal concentration of NaOH for modifying juniper fibre for adsorption of cadmium ions

was carried out by Min et al. (2004). Sodium hydroxide treatment of lignocellulosic materials can cause swelling which

leads to an increase in internal surface area, a decrease in the degree of polymerization, a decrease in crystallinity,

separation of structural linkages between lignin and carbohydrates and disruption of the lignin structure. Sodium hydroxide

is a good reagent for saponification or the conversion of an ester group to carboxylate and alcohol. A maximum

concentration of 0.5 M of NaOH was suitable to carry out saponification process. After base treatment, the maximum

adsorption capacity of cadmium increased by about three times (from 9.18 to 29.54 mg g-1

) compared to untreated juniper

Cadmium Removal from Aqueous Solution by Modified Low Cost Adsorbent(s): A State of the Art 21

fibre despite a decrease in specific surface area for the treated adsorbent.

Modification of Wheat Bran

Wheat bran, a by-product of wheat milling industries proved to be a good adsorbent for removal of many types of

heavy metal ions such as Pb(II), Cu(II) and Cd(II). The application of a strong dehydrating agent like sulfuric acid (H2SO4)

can have a significant effect on the surface area of the adsorbent, which eventually results in better efficiency of adsorption

of copper ions as reported by O¨ zer et al. (2004). It was found that upon treatment with sulfuric acid, wheat bran had a

much higher surface area. The authors suggested that acid treatment caused changes in surface area by increasing the

conversion of macropores to micropores.

The sulfuric acid treated wheat bran for cadmium ion removal from aqueous solution. After 4 h of contact time,

the maximum adsorption capacity that could be achieved for cadmium was 101 mg g-1

at pH5. O¨zer and Pirinc,(2006)

conducted a study on the removal of lead ions by sulfuric acid treated wheat bran. It was reported that maximum lead

removal (82.8%) occurred at pH 6 after 2 h of contact time.

CONCLUSIONS

The main categories of adsorbents are carbon, agricultural wastes, industrial wastes, low grade ores, clays and low

cost synthetic oxides/hydroxides such as iron/manganese/ aluminum. Literature showed that pH is an important factor that

could make a major change in the adsorption capacity. The various adsorption parameters studied to evaluate their effects

on Cd(II) removal efficiency are: contact time, pH, temperature, adsorbate and adsorbent concentrations. It is evident that

low-cost adsorbents have demonstrated outstanding removal capabilities for certain metal ions as compared to activated

carbon. In this review, an extensive list of agricultural wastes as adsorbents including Rice husk, Sawdust (cedrus deodhar

wood), Sawdust (Pinus sylvestris), Walnut sawdust, Juniper fibre, Sugarcane bagasse, Wheat bran, Cassava, tuber bark

waste, Cassava waste, Corncorb, Coirpith, and others has been compiled. Chemically modified agricultural wastes exhibit

higher adsorption capacities than unmodified forms.

Numerous chemicals have been used by many researchers for modifications which include mineral and organic

acids, bases, oxidizing agent, organic compounds, etc. Some of the modified adsorbents show good adsorption capacities

for cadmium. Evaluation of isothermic and thermodynamic parameters has also been outlined as important ones for scale

up and reactor design. A number of modified low-cost adsorbents have been projected as potential candidates for removal

of cadmium from aqueous solution. There is lack of data on regeneration/reuse and safe disposal of loaded adsorbent. More

attention needs to be paid to evaluation of their commercial utilization. A comparison of adsorption efficiency between

chemically modified and unmodified adsorbents was also reviewed.

ACKNOWLEDGEMENTS

Authors are thankful to the Dr D.T. Ingole, Principal, Prof Ram Meghe Institute of Technology and Research for

their encouragement and help during preparation of this manuscript. The authors also thank Director, NEERI, Nagpur and

PKV Akola for permission to collect literature from the library and The Principal, All India Shri Shivaji Memorial

Society’s College of Engineering Pune for permitting to use college laboratory for research work.

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