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Organic geochemistry of the Lower Suban coal seam,South Sumatra Basin, Indonesia: Palaeoecological and

thermal metamorphism implications

Hendra Amijaya 1, Jan Schwarzbauer, Ralf Littke *

Institute of Geology and Geochemistry of Petroleum and Coal, Aachen University, Lochnerstrasse 4-20, 52056 Aachen, Germany

Received 14 June 2005; accepted 31 October 2005

(returned to author for revision 9 August 2005)Available online 19 January 2006

Abstract

Hydrocarbons extracted from the Tertiary age coals from the Lower Suban seam, South Sumatra Basin, Indonesia havebeen investigated using gas chromatography (GC) and combined gas chromatography/mass spectrometry (GC/MS). Lowrank (vitrinite–huminite reflectance 0.41–0.45%) coals from the Tambang Air Laya mine represent different maceralassemblages of an ideal succession of ombrogenous palaeo-peat development in a vertical section. High rank coals (vitr-inite reflectance 1.42–5.18%) from the Suban mine have been thermally metamorphosed by an andesitic intrusion.

Variations in the distributions of n-alkanes, isoprenoids and saturated and aromatic biomarkers in the low rank coalsreflect variations in local source input and palaeomire conditions. Terpenoid biomarkers, such as cadinane- and eudes-mane-type sesquiterpenoids and oleanane- and ursane-type triterpenoids, indicate the predominance of angiosperm plantsin the palaeomire, particularly Dipterocarpaceae. The distribution of hopanoids is affected by the organic facies of the coaland their maturity, and correlates with the palaeomire evolution as derived from petrological studies. Close to the igneousintrusion, rapid thermal stress has destroyed most of the biomarkers, but variations in n-alkane distributions, attributable topalaeomire conditions, remain. Reversals in the trends for molecular parameters based on aliphatic hydrocarbons (n-alkanedistribution and pristane/phytane ratio) and aromatic hydrocarbons (methyl phenanthrenes) with coal rank are observed. 2006 Elsevier Ltd. All rights reserved.

1. Introduction

The dynamics of depositional environments andthe coalification process have been studied using

many physical and chemical methods. Petrographicanalysis is widely applied and gives very usefulinsight into depositional environments of coals(e.g., Diessel, 1992; Calder et al., 1991; and others).However, collaborative study with palaeobotanyand organic geochemistry is needed to elucidatefully the origin of coal (Teichmüller, 1989). A widevariety of organic geochemical indicators reflect pal-aeoenvironmental and palaeoecological conditions(see for example Tissot and Welte, 1984; Peters

0146-6380/$ - see front matter 2006 Elsevier Ltd. All rights reserved.

doi:10.1016/j.orggeochem.2005.10.012

* Corresponding author. Tel.: +49 241 8095748; fax: +49 2418092152.

E-mail address: [email protected] (R. Littke).1 Present address: Department of Geological Engineering,

Gadjah Mada University, Jalan Grafika 2, Yogyakarta 55281,Indonesia.

Organic Geochemistry 37 (2006) 261–279

www.elsevier.com/locate/orggeochem

OrganicGeochemistry

mailto:[email protected]:[email protected]

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and Moldowan, 1993; Hunt, 1996). Biological mar-ker (biomarker) analysis can provide clues aboutenvironmental conditions and botanical and bacte-rial input to the paleomire and has been appliedto many coal deposits from different areas and ages

it has also been applied to recent peat deposits thatmay act as analogues for ancient coal-forming mires(e.g., Dehmer, 1993, 1995; Jiamo et al., 1990; Bech-tel et al., 2003; and many others).

This study deals with the organic geochemicalcharacterization of the Tertiary Lower Suban coalseam in the South Sumatra Basin, Indonesia,which is one of the important oil and coal produc-ing sedimentary basins in Indonesia. Several stud-ies have characterized the coal in detail (Daulayand Cook, 1988; Anggayana, 1996; Daulay et al.,2000; Pujobroto, 2000; Pujobroto and Hutton,

2000; Nas and Pujobroto, 2000). The purpose of this study was to compare the molecular character-istics of the coal with petrographical data describedin detail by Amijaya and Littke (2005) and todeduce information about the palaeoecologicalconditions.

Another important aspect is that thermal alter-ation affects the molecular composition of coal(e.g., Hayatsu et al., 1978; Radke et al., 1982; Dzou

et al., 1995). The heating of organic-rich sedimentsis not always caused by regional basin subsidence,but can also be initiated by igneous activity. Theeffect of igneous activity on the molecular composi-tion of different types of organic matter has become

the subject of many studies (e.g., Raymond andMurchison, 1992; Farrimond et al., 1999; Meyersand Simoneit, 1999). In this study, we examine theeffects of andesitic intrusions on Lower Tertiarycoals from the South Sumatra Basin.

2. Geological background

The Lower Suban coal seam is part of the lowerMPa (Middle Palembang ‘a’), member of the LateMiocene–Early Pliocene Muara Enim Formation(MEF) in the South Sumatra Basin, Indonesia

(Fig. 1), a back-arc basin formed during the pre-Tertiary and early Tertiary (de Coster, 1974; Dalyet al., 1987). Boyd and Peacock (1986) reported thatthe MEF was deposited as a part of a humid tropi-cal deltaic system. The detailed aspects of tectonichistory and stratigraphy of the basin are given inAdiwidjaja and de Coster (1973), de Coster (1974),Gafoer and Purbohadiwidjoyo (1986), Daly et al.(1987) and Darman and Sidi (2000).

Fig. 1. Geological map and general stratigraphy of Tanjung Enim area (modified from Bamco, 1983 and Gafoer et al., 1986). Brokenrectangles show location of main coal fields. The position of Tanjung Enim in the South Sumatra Basin is displayed on the inserted

location map.

262 H. Amijaya et al. / Organic Geochemistry 37 (2006) 261–279

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The economically valuable coal seams (Mangus,Suban and Petai) crop out mostly in the TanjungEnim area. The Suban seam splits into two: theUpper Suban (also known as Suban B1) and theLower Suban (Suban B2) seams. The thickness of

the Lower Suban seam varies between 2 and 3 m.In this area, the coal-bearing strata were subjectedto invasion by plug-like masses of basaltic andesite(Iskandar, 1994) that are presumed to be of Pleisto-cene to early Quaternary age (Gafoer and Purboh-adiwidjoyo, 1986; Darman and Sidi, 2000). Theintrusions caused local thermal metamorphism of the strata and increased the rank of the coals fromlignite through to anthracite in some areas.

3. Samples and methods

3.1. Samples

Coal samples from the Lower Suban seam werecollected from two active surface mines, TambangAir Laya (TAL) and Suban (SUB), situated in theTanjung Enim area (Fig. 1). Random vitrinite(huminite) reflectance (VR

r) measurements of sam-

ples from TAL range between 0.41% and 0.45%,characteristic of low rank coal (in this case lignite)with no sign of extreme heating from the intrusion.In contrast, thermally metamorphosed coals from

SUB show high random vitrinite reflectance values(VR

r) up to 5.18%.

Four samples from the Lower Suban seamfrom TAL were examined. These contain differentmaceral assemblages representing an ideal verticalsuccession of ombrogenous palaeo-peat develop-ment. From base to top, the seam is composed

of humodetrinite-liptinite-rich coal, overlain byhumotelinite-rich and humocollinite-rich coal andfinally humodetrinite-rich coal (Amijaya and Lit-tke, 2005). The petrographical composition of the low rank coals from TAL is presented inTable 1.

Four samples of varying rank were taken fromSUB. These coals were thermally metamorphosedas the Lower Suban seam was penetrated by theandesitic sill. One sample was taken directly atthe contact to the sill. Two were sampled 1.5 and2.5 m above the sill. One was collected at a distance

of approximately 100 m in a horizontal directionfrom the intrusion outcrop along the strike. Thecomposition of the thermally metamorphosed coalis dominated by homogenized vitrinite, althoughthe texture of some vitrinite is still recognizable.Liptinite macerals are largely absent. Inertinite usu-ally presents an unaltered structure, although it isdifficult to recognize it in the coal with high vitri-nite reflectance. The typical microstructure of natu-ral coke (mosaic structure) is recognizable in thesample with the highest reflectance. Table 2 shows

the petrographical characteristics of the high rankcoals.

Table 1Petrographic composition of low rank coals from Lower Suban seam at Tambang Air Laya (TAL)

Samplea VRr (%) Huminite (vol.%) Liptinite (vol.%) Inertinite (vol.%) Mineral matter (vol.%) Maceral assemblageb

02/767 0.45 78.6 18.6 2.3 1.0 Humodetrinite-rich02/769 0.42 73.7 23.2 2.8 0.4 Humocollinite-rich02/771 0.44 85.9 11.6 1.6 1.0 Humotelinite-rich02/773 0.41 34.7 50.8 13.6 1.6 Humodetrinite–liptinite-rich

a Listed from top to base of seam.b Detailed description in Amijaya and Littke (2005).

Table 2Petrographical composition of high rank coals from Lower Suban seam at Suban (SUB)

Sample VRr

(%)Vitrinite(vol.%)

Liptinitea

(vol.%)Inertinite(vol.%)

Mineral matter(vol.%)

Coke mosaicstructure (vol.%)

Distance to intrusion

03/1123 1.42 91.8 0.4 5.6 2.2 – 100 m from contact inhorizontal direction

03/1143 2.09 90.4 1.2 6.8 1.6 – 2.5 m above03/1145 2.55 87.0 0.4 10.6 2.0 – 1.5 m above03/1113 5.18 82.4 – 0.6 14.6 2.40 Directly at contact

a Trace of liptinite is identified as meta-liptinite (altered liptinite with very high reflectance).

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3.2. GC and GC/MS

Coal powder (ca. 10 g) was extracted in a Soxhletapparatus for 24 h using an azeotropic mixture of acetone (47 vol.%), methanol (23 vol.%) and chloro-

form (30 vol.%). Solvent was removed with a rotaryevaporator. The extracts were separated using col-umn chromatography over activated silica gel andeluted sequentially into six fractions using n-pentane(fraction 1), n-pentane/CH2Cl2 (95/5 v/v, fraction2), n-pentane/CH2Cl2 (90/10 v/v, fraction 3), n-pen-tane/CH2Cl2 (40/60 v/v, fraction 4), CH2Cl2 (frac-tion 5) and methanol (fraction 6). Details of theprocedure are described elsewhere (Franke et al.,1995; Schwarzbauer et al., 2000). In this study, onlythe first, second, and fourth fractions were analyzed.

GC was carried out with a Carlo Erba 8000 gas

chromatograph equipped with a 30 m · 0.25 mmID · 0.25 lm film Zebron – ZB 5 fused silica col-umn. The oven temperature was programmed from60 to 300 C at a rate of 3 C/min, with a 20 min iso-thermal period at 300 C. Injection was performedin the split/splitless mode with a splitless time of 60 s. Hydrogen was used as carrier gas (injectiontemperature: 270 C). GC/MS analysis was carriedout using a Finnigan MAT 8222 mass spectrometerlinked to a HP 5890 gas chromatograph. A30 m · 0.25 ID · 0.25 lm film Varian CP Sil –

8CB fused silica column was used. Helium was usedas carrier gas. The temperature programme was asdescribed above. For low resolution mass spectra,the spectrometer was operated at a resolution of 1000 in the EI+ mode (70 eV); the source tempera-ture was 200 C, with scanning from 35 to700 amu at a rate of 1 s/decade and an inter-scantime of 0.1 s.

4. Results

4.1. Molecular composition of low rank coal extracts

4.1.1. n-Alkanes and isoprenoids

The n-alkanes in the low rank coals range from C13to C33 (Fig. 2). Unimodal distributions were observedfor the humotelinite-rich coal (maximum at n-C27)and humodetrinite–liptinite-rich coal (maximum atn-C25). The second type of n-alkane is bimodal,clearly recognized in the humocollinite-rich coal.The first maximum occurs at n-C14 and the long chainn-alkanes exhibit a maximum at n-C24. It is notewor-thy that the n-alkane pattern of humodetrinite-rich

coal maximizes at n-C14, n-C22 and n-C25.

The long chain n-alkanes comprise more than50% of the total n-alkanes in the low rank coals,which is characteristic of their low thermal matu-rity. Except for the extract from the humodetri-nite–liptinite-rich coal, the long chain n-alkanes

exhibit an odd predominance, with Carbon Prefer-ence Index (CPI) values greater than 1 (Table 3).If the CPI is calculated on the full range of n-alk-anes, the values are close to 1. The samples are alsocharacterized by low LHCPI values (

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Humodetrinite-rich

Humocollinite-rich

Humotelinite-rich

Humodetrinite-

liptinite-rich

Retention time

n-C14

n-C14

n-C22

n-C24

n-C27

n-C25

Pr

Pr

Pr

Pr

Ph

Ph

Ph

Ph

Np

Np

Np

n-C14ib

ib

ia

ib

Fig. 2. Mass chromatograms of m/z 57 for aliphatic fraction of low rank coals (VRr = 0.41–0.45%) showing n-alkanes and acyclic

isoprenoids. ia = 2,6,10-trimethylundecane; ib = 2,6,10-trimethyltridecane; Np = norpristane; Pr = pristane; Ph = phytane.


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Table 3

Molecular parameters used for palaeoenvironment and maturity assessment

Sample CPI (BE)a CPI (H)b CPI Allc LHCPId Pr/Ph Pr/n-C17 Ph/n-C18 OleananeIndexe

22S/(22S+22R)Homohopanef

T s/(T s+T m)

Low rank

02/767 1.9 1.5 1.2 0.5 14.7 24.4 1.5 0.2 0.3 0.5 02/769 1.7 1.4 1.2 0.8 11.8 19.1 1.5 0.3 0.4 0.4 02/771 2.2 1.8 1.2 1.2 18.2 21.2 1.1 0.3 0.3 0.5 02/773 0.8 0.7 0.8 0.4 7.1 8.4 0.8 0.2 0.4 0.5 High rank

03/1123 1.1 1.0 1.0 1.7 4.4 0.8 0.2 n.d. n.d. n.d. n03/1143 1.4 1.1 0.9 5.3 4.6 0.5 0.2 n.d. n.d. n.d. n03/1145 1.3 1.1 1.0 1.8 7.0 1.6 0.3 n.d. n.d. n.d. n03/1113 1.1 1.0 1.0 6.7 7.2 0.1 0.02 n.d. n.d. n.d. n

Note: n.d., not detected.a CPI according to Bray and Evans (1961) CPI ¼ 1=2 C25þC27þC29þC31þC33C24þC26þC28þC30þC32 þ

C25þC27þC29þC31þC33C26þC28þC30þC32þC34

.

b CPI according to Hunt (1996) CPI ¼ ð%C25C33oddÞþð%C23C31oddÞ2ð%C24C32evenÞ .

c CPI of all n-alkanes, calculated according to Marzi et al. (1993) CPI ¼

Pm

i¼nC2iþ1þ

Pmþ1

I ¼nþ1C 2iþ1P

mþ1

I ¼nþ1C2i

; n = starting n-alkane divided by 2; m = endd LHCPI ¼ C17þC18þC19C27þC28þC29 (Littke et al., 1998).

e Oleanane Index ¼ 18að H Þþ18bð H Þoleanane17að H Þ;21bð H Þhopane (see Peters and Moldowan, 1993).

f 22S/(22S+22R) ratio for C31-homohopane (see Peters and Moldowan, 1993).

g MPRðMethylphenanthrene RatioÞ ¼ ½2MP½1MP (Radke et al., 1982).

h MPIðMethylphenanthrene IndexÞ ¼ 1:5ð½2MPþ½3MPÞ½ P þ½1MPþ½9MP (Radke et al., 1982).

i

[1-MP]/[9-MP] ratio (Alexander et al., 1992).

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Retention time

Humodetrinite-rich

Humocollinite-rich

Humotelinite-rich

Humodetrinite-

liptinite-rich

A

B

B

B

B

E

E

E

C

DC

CE

F

G

H

I

J

F

G

H I J

F

G

HI

J

F

G

H

I

J

Fig. 3. Some biomarkers in total ion chromatograms for aromatic fraction of low rank coals. Annotations correspond to Table 4.


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1985; Rullkötter et al., 1994). The prominent com-pounds identified in the m/z 410 chromatogramare olean-13(18)-ene, oleane-12-ene, oleane-18-ene,and urs-12-ene; 18a-oleanane, which probably coe-lutes with 18b-oleanane, is also recognizable in the

m/z 412 chromatogram (Fig. 4). Elution of 18a- +18b-oleanane with lupane is possible (see Nytoftet al., 2002). However, a clear indication of the pres-ence of lupane is not recognised. The aromatic pen-tacyclic triterpenoids of the oleanane and ursanetype are found mostly in the form of alkylated-tetra-hydro- or octahydropicenes (Fig. 3).

Steroid compounds do not occur, which is consis-tent with observations by Anggayana (1996) on sev-eral Indonesian Tertiary coals and coals in general(see Chaffee et al., 1986; Wang and Simoneit,1990). However, some recent studies by Lu and

Kaplan (1992) and Bechtel et al. (2003) have indi-cated the occurrence of steroid compounds in somecoals. Chaffee et al. (1986) reasoned that the absenceof steroids may be due to preferential removal orincorporation into the soluble matrix of compo-nents during diagenetic transformation of coal. Itis also possible that sterols were either absent fromthe starting material or have not yet been convertedto steranes or sterenes (Lu and Kaplan, 1992).

4.1.4. Hopanoids

The hopanoids are characterized by the presenceof a series of hopanes from C27 to C33, with bisno-rhopanes C28 being absent (see Fig. 5, based onretention time and mass spectral data published by

Seifert and Moldowan, 1978; Philp, 1985; Lu andKaplan, 1992). C2717a(H)-trisnorhopane (T m) andits isomer 18a(H)-trisnorneohopane (T s) are pres-ent. The value of the T s/(T s + T m) ratio rangesbetween 0.43 and 0.50.

The predominant hopanoid in the low rank TALcoals is C31 17a(H)-homohopane. The presence of C31 hopanes in high concentrations is characteristicof many peats and coals (see for example Lu andKaplan, 1992; Dehmer, 1993, 1995; Anggayana,1996; Bechtel et al., 2003). Both epimers (22R and22S) of C31 17a(H)-homohopane occur. The 22S/

[22S+22R] ratio ranges between 0.3 and 0.4, consis-tent with low maturity sediments and well belowthe equilibrium value (approximately 0.6) thatoccurs at a vitrinite reflectance of around 0.5– 0.6% (see Waples and Machihara, 1990; Petersand Moldowan, 1993). The occurrence of 17b(H),21(b)-hopane is consistent with the low maturityof the TAL coals (Ensminger et al., 1974; Volkmanet al., 1983).

410

412

1

2 3

4

5

*

Fig. 4. m/z 410 and 412 chromatograms for sample 02/773 (humodetrinite/liptinite-rich coal) showing typical sesquiterpenoid distributionfor low rank coal: 1 = olean-13(18)-ene; 2 = olean-12-ene; 3 = olean-18-ene; 4 = urs-12-ene; 5 = 18 a(H) + 18b(H)-oleanane; * = 17a(H),

21b(H)-hopane.


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4.2. Molecular composition of high rank coal extracts

4.2.1. Aliphatic hydrocarbons

High rank coals from the Lower Suban seam inthe Suban area were subjected to varying degreesof thermal stress by the intrusion of the andesiticsill. Extracts exhibit various n-alkane distributionsalthough the concentration is low (Fig. 6). Those

with unimodal distributions are exhibited by the

coal at VRr = 1.42% (n-alkane max. at n-C16) and

by the coal with the highest VRr (5.18%, n-alkane

max. at n-C17). Coals with intermediate VRr valuesare characterized by bimodal distributions.

The relative abundance of light n-alkanes toheavy n-alkanes also exhibits a broad variation inthe high rank Suban area coals. The LHCPI valuesvary between 1.7 and 6.7 and do not show any par-ticular pattern (Table 3 and Fig. 7). The CPI of highmolecular weight n-alkanes and the full range of n-alkanes is 1, consistent with high thermal maturity.

The pristane/phytane ratios are low compared tovalues seen in the lower rank TAL coals (Fig. 7).The Pr/nC17 and Ph/nC18 ratios of the low rankcoals are appreciably higher than those of the highrank coals. Other smaller acyclic isoprenoids, suchas norpristane or farnesane, are present in the coalwith VR

r = 1.42%. The saturated cyclic isoprenoids

are absent, except in the coal with VRr = 1.42%, for

which sesquiterpenoids are still present but are notidentifiable. The cyclic isoprenoids appear to havebeen aromatized completely as a result of extreme

heating by the intrusion.

Retention time

Humodetrinite-rich

Humocollinite-rich

Humotelinite-rich

Humodetrinite-

liptinite-rich

fa b

c

d

e g

h

ik

l

fa b

c

d

eg

h

i

k

l

fa b

c

d

e

g

h

i k l

fa b

c

d

eg

h

ik

l

Fig. 5. Hopanoid distribution according to m/z 191 chromato-gram for low rank coals (for peak assignment see Table 4).

Table 4Peak assignment for biomarkers in aromatic fraction (Fig. 3) andhopanoids in aliphatic fraction (Fig. 5) of low rank coal fromTAL

Peak Compounda

Aromatic hydrocarbons

A IoneneB PentamethylindaneC 5,6,7,8-TetrahydrocadaleneD CalameneE CadaleneF 2,2,4a,9-Tetramethyl-1,2,3,4,4a,5,6,14b-octahydropiceneG 1,2,4a,9-Tetramethyl-1,2,3,4,4a,5,6,14b-octahydropiceneH 2,2-Dimethyl-1,2,3,4-tetrahydropiceneI 1,2,9-Trimethyl-1,2,3,4-tetrahydropiceneJ 2,2,9-Trimethyl-1,2,3,4-tetrahydropicene

Hopanoids

a 18a(H)-22,29,30-Trisnorneohopane (T s)b 17a(H)-22,29,30-Trisnorhopane (T m)

c 17a(H),21b(H)-30-Norhopaned 17b(H),21a(H)-30-Normoretanee 17a(H),21b(H)-Hopanef 17b(H),21a(H)-Moretaneg 17a(H),21b(H)-30-Homohopane (22S)h 17a(H),21b(H)-30-Homohopane (22R)i 17b(H),21b(H)-Hopane j 17a(H),21b(H)-30,31-Bishomohopane (22S)k 17a(H),21b(H)-30,31-Bishomohopane (22R)l 17b(H),21a(H)-30,31-Bishomomoretane

a Identification based on relative retention times and publishedmass spectral data.


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Retention time

VRr = 1.42%

VRr = 2.09%

VRr = 2.55%

VRr = 5.18%

n-C16

n-C16

n-C15

n-C17

n-C23

n-C23

Pr

Pr

Pr

Pr

Ph

Ph

Ph

Ph

Fig. 6. Total ion chromatograms for aliphatic fraction of high rank coals.


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4.2.2. Aromatic hydrocarbons

Various aromatic hydrocarbon compounds occurin the thermally metamorphosed coals. Distri-butions of the isomers of the main compounds(methylnaphthalene, dimethylnaphthalene, trimeth-ylnaphthalene, phenanthrene, methylphenanthrene,dimethylphenanthrene, trimethylphenanthrene) arepresented in Fig. 8.

A reversal pattern is shown by the relative abun-dance of the isomers of naphthalene relative tophenanthrene. In general, there is a decrease in theabundance of naphthalenes relative to the phe-nanthrenes with increasing rank for VR

r = 1.42–

2.55%. However, in the coal taken directly at theintrusion contact (VR

r = 5.18%), the naphthalene

isomers are more abundant.Several maturity indices have been formulated

based upon the distribution of methyl-substitutedaromatic compounds. The MPR (methylphenanth-rene ratio), MPI (methylphenanthrene index) bothproposed by Radke et al. (1982) and the 1-MP/9-

MP ratio (Alexander et al., 1992) values (Table 3

and Fig. 9) vary considerably in the low rank coal.MPR and MPI increase with rank before decreasingat very high rank (above VR

r 2.5%), whereas the

1-MP/9-MP value of the high rank coals is invariateat about 1.2–1.3 (Table 3 and Fig. 10).

5. Discussion

5.1. Palaeoecological and palaeoenvironmental

conditions

The formation of palaeo-peat is known to berelated to the environmental conditions of the pal-aeomire. Petrographical analysis of the LowerSuban seam had confirmed the development of araised palaeo-peat bog (Amijaya and Littke, 2005).The organic geochemical analysis was intended to

provide information on plant input, bacterial activ-ity and the interaction with the palaeoenvironment,which basically encompass the palaeoecologicalconditions for the coal precursor.

It is well known that the dominance of longover short-chain n-alkanes is typical for immaturecoals composed of higher land plant organic mat-ter (Wang and Simoneit, 1990; Stout, 1992; Zhanget al., 1993; Petersen et al., 2001; Bechtel et al.,2003) and, specifically, cuticular waxes (Eglintonand Hamilton, 1967). The bimodal distribution

could indicate a mixture of terrigenous higher landplant material and an algal/bacterial source(Moldowan et al., 1985). However, abundant algalmaterial was not microscopically identified (Ami-

jaya and Littke, 2005). The abundance of smallern-alkanes is likely attributable to microbialactivity.

The isoprenoids are mainly derived from the phy-tol side chain of chlorophyll in phototrophic organ-isms although other sources such as archaebacteriaare also known (Volkman and Maxwell, 1986 andreferences therein). The presence of a C

16-isopren-

oid in high concentration in humodetrinite- andhumocollinite-rich coals supports the possibility of enhanced microbial activity in the top section of the palaeo-peat. In this case, the bacteria may eitheract as a direct source of acyclic isoprenoids or as adegradation agent.

The biomarker composition of the coals indicatesthat the palaeo-peat was formed from angiospermvegetation. As mentioned above, cadinane andeudesmane dominate the saturated sesquiterpanes.Cadinane is regarded as the product of depolymer-

ization and subsequent hydrogenation of polycadin-

0

5

10

20

25

30

VR r (%)

15

Pr/Ph

Pr/ n -C17

Ph/ n -C18

R a t i o

0

1

2

3

4

5

6

7

0 3 5

VR r(%)

R a t i o

CPI(BE)

CPI(Hunt)

CPI All

LHCPI

21 4 6

0 3 521 4 6

a

b

Fig. 7. Change in: (a) CPI and (b) Pr/Ph, Pr/nC17 and Ph/nC18with increasing maturity indicated by random vitrinitereflectance.


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ene, a compound found in angiosperm dammarresin, most of all of the Dipterocarpaceae family thatinhabits Southeast Asia (Aarssen et al., 1992, 1994).This finding agrees with the pollen analysis that

identifies Dipterocarpaceae in Tertiary coal and

recent peat of Indonesia. One of its genera, Shorea,is a typical plant found in modern ombrogenoustropical lowland peat swamps in Indonesia, espe-cially Sumatra and Kalimantan (Anderson and

Müller, 1975; Morley, 1981; Demchuck and Moore,

Retention time

VRr = 1.42%

VRr = 2.09%

VRr = 2.55%

VRr = 5.18%

MN

DMP

TMP

MPP

TMN

DMN

MN

DMP

TMP

MPP

TMN

DMN

MN

DMP

MP

P

TMN

DMN

DMP

TMP

MP

P

TMN

DMN

Fig. 8. Total ion chromatograms for aromatic fraction of high rank coals and indication of position of some important aromatichydrocarbons. MN = methylnaphthalene; DMN = dimethylnaphthalene; TMP = trimethylnaphthalene; P = phenanthrene; MP = methyl-phenanthrene; DMP = dimethylphenanthrene; TMP = trimethylphenanthrene.


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1993). The presence of a sesquiterpanoid with aeudesmane skeleton, probably 4b(H)-eudesmane, isalso consistent with an input from higher landplants (Alexander et al., 1984).

The precursors of the aromatic sesquiterpenoidsin the coals (cadalene, tetrahydrocadalene andcalamene) are found mostly in angiosperm dammar

resin (Bendoraitis, 1974; Simoneit and Mazurek,

1982; Wang and Simoneit, 1990; Aarssen et al.,1992). Depolymerization of polycadinene duringcatagenesis initiates an aromatization that leads tothe formation of these compounds (Aarssen et al.,1992).

The ionene (1,1,6-trimethyltetralin) and 1,6,8-trimethyltetralin are probably derived fromdegraded and cyclized carotenoids (Wang and Sim-

oneit, 1990). Carotenoids have been proposed toconstitute sporopollenins derived from some higherplant pollen and ionene was identified in pyrolysatesof sporopollenins derived from some higher plantpollen and spore coal (Achari et al., 1973).

Abietane is found in the humotellinite-rich coal.Diterpenoids are predominant constituents of higher plant resins, mostly from gymnosperms (seeSimoneit, 1986; Chaffee et al., 1986; Killops et al.,1995; Otto et al., 2005), though diterpenoids arealso found in some species of angiosperms, such asthe family Burseraceae (Sukh Dev, 1989). Com-pounds with an abietane skeleton are found mostlyin conifer resins and lipids in form of abietic acid,abietinol or ferruginol (Laflamme and Hites, 1979;Sukh Dev, 1989).

The absence of diterpenoids from most of thesamples can be correlated with an absence of gym-nosperm precursors at the time of deposition, sinceangiosperms are the predominant plants in Tertiarycoals and recent ombrogenous peats from theMalay-Indonesian region (Anderson and Müller,1975; Morley, 1981; Demchuck and Moore, 1993).

However, Anderson and Müller (1975) identified

Retention time

VRr = 1.42%

VRr = 2.09%

VRr

= 2.55%

VRr = 5.18%

VRr

= 0.44%3-MP

2-MP

9-MP

1-MP

3-MP

2-MP

9-MP

1-MP

3-MP

2-MP

9-MP1-MP

3-MP

2-MP

9-MP 1-MP

3-MP2-MP

9-MP1-MP

Fig. 9. Methylphenanthrene distribution in coal samples of different rank.

0

1

2

3

4

5

6

7

8

0 2 5

VRr (%)

1MP/9MP

MPR

MPI

R a t i o

1 3 4 6

Fig. 10. Change in 1-MP/9-MP, methylphenanthrene ratios andmethylphenanthrene index with increasing thermal maturity

indicated by random vitrinite reflectance of coals.


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some conifer pollen grains (Dacrydium and Podo-carpus) in peat deposits and Burseraceae pollengrains in clay underlying a peat deposit in NW Kali-mantan. A species of Dacrydium is prominent in apeat swamp forest in one locality in that area.

Although there is no palynological evidence in thestudied area, the occurrence of diterpenoids in oneof the coals is likely due to such local variations inbiotic input at the time of deposition.

The role of angiosperms as palaeo-peat-formingvegetation is also revealed by the occurrence of tri-terpenes, especially the defunctionalized, unsatu-rated and monoaromatic oleanane or ursane,which are found mostly in the Dicotylodonea, angio-sperm dicots. Only a few gymnosperm species con-taining these compounds are known (Simoneitet al., 1986; Sukh Dev, 1989; Otto et al., 2005; Stefa-

nova et al., 2005). Ten Haven et al. (1992) suggestedthat olean-12-ene and urs-12-ene are mainly alter-ation products of b- and a-amyrin. Oleananes areformed through diagenetic and catagenetic alter-ation of various 3b-functionalized angiosperm trit-erpenoids (see Rullkötter et al., 1994; Murrayet al., 1997) or the catalytic hydrogenation of olean-ene (Rullkötter et al., 1994). Des-A-lupane, the onlysesterterpenoid in significant concentration, hasbeen considered a product of photochemical or pho-tomimetic degradation at ring-A, commencing with

the oxygen functionality at C-3 of certain triterpe-noids (but not hopanes) from higher plants (Corbetet al., 1980; Simoneit, 1986).

Aromatic pentacyclic triterpenoid compoundswith a picene structure are considered biomarkersfor angiosperms, since they have been identified inlignite from angiosperms (Stout, 1992). These struc-tures may result from the microbial aromatizationof triterpenoids (Wakeham et al., 1980; Stout,1992). Dehmer (1988) identified several compoundswith the same structures in peat deposits in Indone-sia, indicating that the dehydrogenation of triterpe-noids does not require long periods of time or hightemperature.

The presence of hopanoids points to microbialinput due to their primary origin (Simoneit, 1986).The major hopanoid, 17a(H)-homohopane, resultsfrom the oxidative reactions and subsequent decar-boxylation of bacteriohopanetetrol and other pre-cursors; and a,b-C31-hopanes are often the majorhopanes in coals derived from peat deposited inacidic environments (Dorsselaer et al., 1977). Thisfinding agrees with the fact that an acidic environ-

ment is typical for domed peat deposits in Indonesia

(Neuzil et al., 1993; Dehmer, 1993). Noteworthy isthe dominance of 17a(H),21b(H)-30-norhopane inhumotelinite-rich coal. Lu and Kaplan (1992)observed an enrichment in norhopanes with increas-ing temperature. However, in this TAL low rank

coal, the variation in hopane distribution is likelysource dependent.Dydik et al. (1978) proposed that Pr/Ph values

reflect the redox conditions during organic matterdeposition. Accordingly, the humodetrinite-, humo-collinite-, and humotelinite-rich coals (higher Pr/Ph)were developed under more oxic conditions than thehumodetrinite-liptinite-rich coal, which is accept-able since the humodetrinite/liptinite-rich is a typi-cal coal facies for planar-topogenous palaeomireswhereas the other facies are typical for domed-ombrogenous palaeomires in the area (Amijaya

and Littke, 2005). Similar variations in Pr/Ph wereobserved by Bechtel et al. (2002, 2003) for ligniteseams in Austria and Slovenia. Other interpreta-tions of Pr/Ph ratios (e.g., Ten Haven et al., 1987)take other sources into account but are probablyless relevant in the case of peat and coal. The roleof liptinite macerals to reduce the value of Pr/Phis also a matter of debate, because liptinite-richcoals could have a wide range of Pr/Ph ratios (seePüttmann et al., 1986).

The influence of maturation on the variability of

Pr/Ph values can also be ruled out in this low rankcoal, because the samples are at the same maturitylevel (VR

r = 0.41–0.45%). Nevertheless, a bacterial

origin of phytane (Volkman and Maxwell, 1986)can not be excluded. High pristane/n-C17 ratios(>1) are indicative of sediment deposition in inlandpeat swamp environments (Lijmbach, 1975), whichagrees with the depositional environment of thestudied coals (Boyd and Peacock, 1986; Amijayaand Littke, 2005).

The T m/T s ratio may reflect the redox potentialof the palaoenvironment with higher T

m/T

s ratios

indicating oxic conditions during sedimentation(Moldowan et al., 1986). This explanation is consis-tent with the Pr/Ph ratio of the TAL coal samples asthe coals with higher T m/T s ratios are those thatwere deposited in the upper part of the ombroge-nous palaeomire under prolonged oxic conditions.However, it is also possible that the small variationin the ratio of T s to T m is related to the difference inthe maceral composition of the coals. The highestratio is found in the humocollinite-rich coal, whichis composed mostly of corpohuminite (Amijaya

and Littke, 2005). Corpohuminite originates from


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tannins, primary cell excretions that later are con-verted to phlobaphenes by oxidation or condensa-tion (Taylor et al., 1998; Sýkorová et al., 2005).The process of corpohuminite formation could pos-sibly drive an advance production of T m.

5.2. Effect of thermal metamorphism caused by

intrusion

Varying degrees of thermal stress resulting fromthe andesitic intrusion have changed the n-alkanedistributions. A reversal pattern of n-alkane distri-bution from unimodal to bimodal and back to uni-modal with increasing maturity is noted. George(1992) observed a similar phenomenon in a shalehorizon intruded by a sill in Scotland and suggestedthat the unusual modification of n-alkane distribu-

tions is probably due to the rapid heating of imma-ture organic matter. The result of our study on SUBcoals supports this suggestion.

However, the influence of precursor material asseen in the lower rank TAL samples should not beneglected. Unfortunately, such influence can notbe recognized microscopically because the maceralsin the high rank coals are homogenized.

Heating by the intrusion greatly lowers the ratioof pristane to phytane compared to values seen inthe lower rank TAL coals (Fig. 7). The Pr/Ph ratio,

however, does not directly correlate with thermalexposure as it first decreases then increases at thehighest level of maturation. Some studies indicatethat the Ph/Pr ratio reaches a maximum at mediumrank (VR

r = 0.7–1.0%, Radke et al., 1980; Littkeet al., 1990). The trend in the ratio for the Subanarea coals may be typical for rapid coalification of low rank coal caused by the igneous intrusion,which was also found by Norgate et al. (1999) in astudy of New Zealand coals.

As presented in Fig. 8, a decrease in the abun-dance of the methyl-substituted phenanthrenes rela-tive to phenanthrene occurs with increasing rank, inagreement with the transformation pattern of tricy-clic diterpenoids with increasing coal rank asdescribed by Hayatsu et al. (1978). As mentionedabove, a reversal pattern is shown by the relativeabundance of the naphthalene isomers relative tophenanthrene. It should be noted that, for type IIIkerogen, the change in distribution of naphthaleneisomers with increasing rank is a less reliable ther-mal indicator than that for phenanthrene isomers(Radke et al., 1986; Raymond and Murchison,

1992).

The result of MPR change with rank is basicallyin agreement with the study by Radke et al. (1984),which inferred a gradient reversal between 1.7 and2.5% VR

r for MPR. However, unlike the data from

Radke et al. (1982), which indicated a reversal of

MPI at VRr 1.3%, the reversal in this thermallymetamorphosed coal occurs at higher vitrinitereflectance (above 2.5%). These data support thesuggestions of Raymond and Murchison (1992),indicating that MPI is highly susceptible to differ-ences in heating rate and organic matter type and,thus, is considered an unreliable maturity parame-ter. However, the trend in MPI for the Lower Subancoals is similar to that described by these authors.They also found that rapidly heat-affected organicmatter exhibits a more immature molecular signa-ture than organic matter exposure to normal geo-

thermal gradients at the same vitrinite reflectance.Change in the molecular characteristics of LowerSuban coals caused by rapid heating due to igneousactivity confirms this fact.

In the oil window range, the value of the 1-MP/9-MP ratio for sediment extracts increases with rank(Alexander et al., 1992). Our study shows that thelow rank coals of TAL have a low 1-MP/9-MPratio, even though one sample has an anomalouslyhigh value. The high rank coals from SUB showsimilar values. This observation possibly indicates

that an equilibrium value of the 1-MP/9-MP ratiocan be reached at a certain rank, possibly close toVR

r = 1.4%.

6. Conclusions

A number of conclusions can be drawn from thepreserved biomarkers in the coals and their responseto the thermal metamorphism caused by the igneousintrusion.

(1) The n-alkane distribution is correlated withthe different maceral assemblages in the lowrank coals. It should be noted, however, thatthis distribution could be due to the differentintensity of microbial activity at each part of the palaeomire.

(2) In this case, the pristane/phytane ratio can beused to draw conclusions about the redox con-ditions within the palaeomire, because it isconsistent with the palaeoenvironmental inter-pretation based on maceral assemblages. Thehumodetrinite-liptinite-rich coal, the typical

facies for planar-topogenous palaeomires,


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shows the lowest Pr/Ph ratio in comparison tothe other coal facies, which were deposited indomed-ombrogenous palaeomires (see Ami-

jaya and Littke, 2005).(3) The composition of terpenoid biomarkers

(especially cadinane and eudesmane-type ses-quiterpenoids and oleanane and ursane typetriterpenoids) indicates an abundant contribu-tion of angiosperm plants to the Late Mio-cene/Early Pliocene palaeoecology of thepalaeomire in this area.

(4) The distribution of hopanoids is influenced bythe organic facies of the coal and the maturity.The pattern of the T m/T s ratio reflects the pal-aeomire conditions, since a higher T m/T s ratiois shown by the coals which were more oxi-dized and deposited as the upper part of the

ombrogenous palaeomire. The predominanthopanoids in most of the low rank coals arethe 22R and 22S epimers of 17a(H)-homoho-pane, which is a common characteristic of many peats and coals deposited in acidicenvironments.

(5) There is a reversal pattern in the trends of molecular maturity parameters based on thealiphatic hydrocarbons (n-alkane distributionand pristane/phytane ratio) and the aromatichydrocarbons (methylphenanthrene) with coal

rank. CPI equilibrium at 1 is reached at amaturity with vitrinite reflectance lower than1.4%, whereas the Pr/Ph ratio decreases withthermal maturity but increases again in theanthracite stage. The values of methylphe-nanthrene ratios MPR, MPI, and 1-MP/9-MP vary considerably in low rank coal. Inthe high rank coal, the MPR and MPI increasewith rank before decreasing at very high matu-rity (above VR

r 2.5%). However, the 1-MP/

9-MP ratio of the high rank coals remainsquite constant.

Acknowledgements

The first author is most grateful for financial sup-port provided by the German Academic ExchangeService (DAAD). Coal samples were kindly pro-vided by PT Tambang Batubara Bukit Asam. Tech-nical assistance from R. Meier and E. Eseme withGC-GC/MS analysis is gratefully acknowledged.This paper also benefitted from some suggestions

by B. Krooss. We thank M.A. Kruge, H.I. Petersen

and C.C. Walters for their comments and sugges-tions, which significantly improved the manuscript.

Associate Editor — C.C. Walters

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