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Origin and Secondary Alteration of Coalbed and Adjacent Rock Gases in the Zonguldak Basin, Western Black Sea Turkey

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Origin and Secondary Alteration of Coalbed and Adjacent Rock Gases in the Zonguldak Basin, Western Black Sea Turkey Geochemical Journal, Vol. 41, pp. 201 to 211, 2007 Origin and secondary alteration of coalbed and adjacent rock gases in the Zonguldak Basin, western Black Sea Turkey HAKAN HOSGÖRMEZ¸ Istanbul University, Engineering Faculty, Geology Department, TR-34320, Avcılar, Istanbul, Turkey (Received March 3, 2006; Accepted March 23, 2007) Investigation of molecular and carbon isotopic composition variability of hydrocarbon gases (methane, ethane and propane) has been performed on gases from coal and rock samples from Kozlu district of the Zonguldak Basin in order to ascertain the origin of gases and to explain possible reasons of variations in molecular and isotopic composition. For this purpose, the molecular and isotopic composition of eight headspace and associated gases from coals and adjacent organic rich sediments of two different stratigraphic levels of Kozlu formation in the Zonguldak basin have been determined. Total organic carbon (TOC) measurements and Rock-Eval pyrolysis were performed in order to determine bulk organic geochemical characteristics of the respective intervals. Coal and associated rock samples contain predominantly vitrinite rich type III organic matter with hydrogen indices (HI) up to 162 mgHC/gTOC. The stable carbon isotope ratios (δ13C) of the kerogen vary from –25.52‰ to –28.05‰. All the headspace gaseous hydrocarbons are dominated by methane (>94%). δ13C range for methane, ethane and propane of δ13 δ13 δ13 the headspace samples are defined as; C1: –48.4‰ to –36.3‰, C2: –26.7‰ to –17.5‰ and C3: –31.8‰ to –22.3‰, respectively. Methane isotopic composition and molecular ratios of the gases show that the origin of gases is mainly thermogenic. But admixture of some biogenic gas is also possible. The amount of the biogenic admixture is controlled mainly by cleat/fracture intensity of the coal or rock. The biogenic admixture of methane increases with increasing inten- sity of the rock fractures. In other words, methane isotope composition becomes much lighter with increasing proximity to a fault of to a crushed zone. Isotopic composition of methane and geological history of the basin led to the conclusion, that biogenic component is related with secondary bacterial gas generation. Ethane is unexpectedly heavier than the propane in all of the analyzed samples. It becomes heavier in samples particu- larly from the Mileopera seam, which is intensively cleated. The gases with a negative stable carbon isotope sequence of δ13 δ13 C2 > C3 may possibly imply a microbial alteration. Respective isotope values of headspace and associated gases can also be influenced additionally by desorption process, which is caused by uplift of the basin during the last 42 million years. Keywords: coal-bed gas, isotopic composition, secondary bacterial gas, microbial oxidation, western Black Sea Yalçın, 2000), amount and molecular composition of coal- INTRODUCTION bed gas in various coal seams (Ho¸sgörmez, 1996; The coal-bearing Carboniferous sequence of the Ho¸sgörmez et al., 1997, 1998). Zonguldak Basin is located in Northwestern Turkey on Until now, detailed investigations on isotopic compo- the Black Sea Coast (Fig. 1). The Zonguldak Basin con- sition of coalbed gas in the Carboniferous Zonguldak sists of Carboniferous coal seams which are produced Basin coals are limited. The only one study is carried out since more than 100 years. Consequently, the basin was by Ho¸sgörmez et al. (2002) on the headspace samples studied by several researchers for different reasons: ge- from two boreholes (AK-14 and AK-16) in the Amasra ology (Kerey, 1982), coalbed methane potential (Mann region of the Zonguldak Basin. This study, showed that et al., 1995; Yalçın, 1995, 1997; Yalçın et al., 1994, 2002; isotopically light methane and to a certain degree ethane Harput et al., 1999), source rock potential (Derman and and propane can be related to of an admixture of ther- I˙ ztan, 1997), organic petrography (Karayi˘git, 1989; mogenic and secondary biogenic gas. Karayi˘git et al., 1998), adsorption capacity of coals The objectives of this study are to determine the mo- (Gürdal and Yalçın, 1995; Gürdal, 1998; Gürdal and lecular and isotopic composition of coalbed and adjacent rock gases in the Kozlu district of the Zonguldak basin and to discuss its origin. Furthermore, it is aimed to fig- *e-mail address: [email protected] ure out whether cleat/fracture intensity of coals does in- Copyright © 2007 by The Geochemical Society of Japan. fluence the molecular and isotopic composition of the 201 Fig. 1. Location map of the Kozlu Block (Zonguldak), showing the geological map of the study area and coal operation area in Zonguldak Basin. gases. For this purpose, headspace samples were taken Alacaa˘gzı Formation is conformably overlain by Kozlu from different coal seams of varying cleat intensity and Formation which contains of mostly coal seams. from localities of varying fracture intensity caused by Westphalian-A aged Kozlu Formation is formed by inter- faults. Data obtained from the analyses are used to clas- bedded sandstones, siltstones, mudstones, conglomerates sify the gases, to distinguish their origin and to discuss and coals. The overlying Westphalian B-C aged Karadon possible effects of seconday processes on molecular com- Formation bears a similar succession as the Kozlu for- position and isotope ratios. mation, however with less number of coal seams. They exist more than twenty coal seams such as Mileopera, Çay, and Acılık within the Kozlu formation. Net coal thick- STRATIGRAPHY OF THE COAL SEAMS ness for this stratigraphic sequence ranges from 30 to 32 The oldest unit of the coal bearing sequence of the m across the Kozlu region. Zonguldak Basin Carboniferous is the Visean aged Yılanlı The Carboniferous Alacaa˘gzı, Kozlu and Karadon Formation, which consists of marly and partly dolomitic Formations are unconformably overlain by Cretaceous limestones and carbonaceous shales (Fig. 2). Yılanlı For- units (Fig. 2) (Görür and Tüysüz, 1997; Yılmaz et al., mation is conformably overlain by Alacaa˘gzı Formation. 1997), which generally composed of limestone and Namurian-aged Alacaa˘gzı Formation consists predomi- dolomitic limestone. The Carboniferous units experienced nantly of light-colored fine to medium-grained, two major burial and subsequent uplift-erosion episodes. crossbedded sandstones and siltstones interbedded with These two episodes of burial and subsequent uplift and shale (Yergök et al., 1987; Orhan and Canca, 1989). erosion are typical for the entire region and have remark- 202 H. Ho¸sgörmez Fig. 2. Generalized stratigraphic section of the study area from the Zonguldak Basin. ably controlled the coalification, gas generation, SAMPLES AND METHODS desorption of coal-bed gas within the Carboniferous coals (Yalçın et al., 2002). Samples were taken from coal seams and adjacent Active tectonics during the Paleozoic and Mesozoic rocks present the Kozlu Formation in the Kozlu Coal Dis- in the Western Black Sea region had a major control on trict, Zonguldak (Fig. 1) at eight different points using structural evolution of the basin. East-Northeast/West- headspace cans. During sampling, after the blasting in southwest striking folds and thrusts with a northerly ver- the gallery, aliquots, which were taken from a piece of gence indicating West-Northwest/East-Southeast com- rocks of 4–5 cm thick from fresh rock surfaces, were pression has occurred a as a result of the Hercynian immediately placed in air-tight glass containers. Tap wa- orogeny. The next major tectonism is represented by East- ter was then added until a sufficient space at the top of West striking normal faults in connection with a rift sys- the containers was left for the accumulation of the so- tem during the Albian-Cenomanian (Görür et al., 1993; called “headspace gas”. The samples were preserved in Robinson et al., 1996). Consequently, these faults caused sealed headspace cans (Schaefer et al., 1984). Bacterial fracturing of coal beds and formed suitable pathways for degradation was inhibited by adding benzalkonium chlo- meteoric water flow. ride (Zephirol®). Four of the samples were collected from Origin and secondary alteration of coal gases 203 204 H.Ho¸ Table 1. Isotopic composition and organic geochemical characteristics of the rock and coal samples in the Zonguldak Basin, Turkey sgörmez Age Seam Sample No. Depth Sample Lithology Kerogen isotopic composition TOC Calculated Ro Tmax HI S1 S2 (m) determination ( vs. PDB) (%) (%) (°C) (mgHC/gTOC) (mgHC/gTOC) (mgHC/gTOC) Westphalian HS001 560 Siltstone Siltstone −25.65 13.69 1.08 459 97 80 13220 354 sewer (fractured) Westphalian HS002 560 Siltstone Siltstone −25.52 7.50 1.03 456 106 760 7950 354 sewer (fractured) Westphalian HS003 560 Coal Coal −26.01 72.14 1.10 460 162 5620 116980 354 sewer (uncleated) Westphalian HS004 560 Coal Coal −25.98 69.71 1.10 460 114 3590 79140 354 sewer (uncleated) Westphalian Mileopera HS005 530 Coal Coal −28.05 85.15 1.06 458 131 510 111210 355 sewer (cleated) Westphalian Mileopera HS006 530 Coal Coal −26.95 79.38 1.08 459 137 3177 98785 355 sewer (cleated) Westphalian Mileopera HS007 530 Coal Coal −27.46 82.49 1.10 460 146 3817 115234 355 sewer (cleated) Westphalian HS008 560 Siltstone Siltstone −25.75 21.64 1.08 459 105 905 33773 354 sewer (fractured) lecular compositionandamountofCO todeterminetypeofhydrocarbons,theirmo- detector, 6890N gaschromatograph,equippedwitha(FID)–(TCD) Agilent- ments ofthecoalsampleswerecarriedoutby The headspace andassociatedgasmeasure- two months. was carriedouton“headspacegas”atSTPconditionsafter
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