Stable carbon and hydrogen isotopic characteristics of natural gas from Taibei sag, Turpan-Hami Basin, NW China
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摘要
Turpan-Hami Basin is a major petroliferous basin in China. To date the natural gas exploration is concentrated in the Taibei sag. The origin and source of natural gas in the Taibei sag has long been controversial. To further investigate the origin and source of the natural gas in the Taibei sag, combined with previous studies and the local geological backgrounds, this study collected 23 gas samples from the Baka, Qiuling, Shanshan and Wenmi oil fields in the Taibei sag and analyzed the sample composition, stable carbon and hydrogen isotopes of all the gas samples. The results show that, gases from the four oil fields in the Taibei sag are dominated by hydrocarbon gas and belong to wet gas. Methane accounts for 65.84% to 97.94%, the content of heavy hydrocarbon(C2-5) can be up to 34.98%, while the content of nonhydrocarbon(CO_2, N_2) is trace. The δ~(13) C_1 value is –44.9‰ to –40.4‰, δ~(13) C_2 is –28.2‰ to –24.9‰, δ~(13) C_3 is –27.1‰ to–18.0‰ and δ~(13) C_4 is –26.7‰ to –22.1; while the variation of δD1 is not significant from –272‰ to –252‰, δD_2 is –236‰ to –200‰ and δD_3 is –222‰ to –174‰. Methane and its homologues(C_(2-5)) are characterized by normal stable carbon and hydrogen isotopic distribution pattern, i.e., with the increase of carbon number, methane and its homologues become more and more enriched in 13 C or D(δ~(13) C_1<δ~(13) C_2<δ~(13) C_3<δ~(13) C_4<δ~(13) C_5, δD1<δD_2<δD_3), which is consistent with the carbon and hydrogen isotopic features of typical thermogenic gas. All these results show that the natural gases in the four oil fields are coal-derived gas with low maturity(Ro averaged at0.7%), and are sourced from the Middle-Lower Jurassic coal measure. The hydrogen isotopic data of natural gas are affected by both thermal maturity and the water medium of the environment where source rocks are formed. The hydrogen isotopic data indicate that the source rocks are formed in terrestrial limnetic facies with freshwater. Natural gases from Well Ba23 and Well Ke19 experienced biodegradation in the late stage.
Turpan-Hami Basin is a major petroliferous basin in China. To date the natural gas exploration is concentrated in the Taibei sag. The origin and source of natural gas in the Taibei sag has long been controversial. To further investigate the origin and source of the natural gas in the Taibei sag, combined with previous studies and the local geological backgrounds, this study collected 23 gas samples from the Baka, Qiuling, Shanshan and Wenmi oil fields in the Taibei sag and analyzed the sample composition, stable carbon and hydrogen isotopes of all the gas samples. The results show that, gases from the four oil fields in the Taibei sag are dominated by hydrocarbon gas and belong to wet gas. Methane accounts for 65.84% to 97.94%, the content of heavy hydrocarbon(C2-5) can be up to 34.98%, while the content of nonhydrocarbon(CO_2, N_2) is trace. The δ~(13) C_1 value is –44.9‰ to –40.4‰, δ~(13) C_2 is –28.2‰ to –24.9‰, δ~(13) C_3 is –27.1‰ to–18.0‰ and δ~(13) C_4 is –26.7‰ to –22.1; while the variation of δD1 is not significant from –272‰ to –252‰, δD_2 is –236‰ to –200‰ and δD_3 is –222‰ to –174‰. Methane and its homologues(C_(2-5)) are characterized by normal stable carbon and hydrogen isotopic distribution pattern, i.e., with the increase of carbon number, methane and its homologues become more and more enriched in 13 C or D(δ~(13) C_1<δ~(13) C_2<δ~(13) C_3<δ~(13) C_4<δ~(13) C_5, δD1<δD_2<δD_3), which is consistent with the carbon and hydrogen isotopic features of typical thermogenic gas. All these results show that the natural gases in the four oil fields are coal-derived gas with low maturity(Ro averaged at0.7%), and are sourced from the Middle-Lower Jurassic coal measure. The hydrogen isotopic data of natural gas are affected by both thermal maturity and the water medium of the environment where source rocks are formed. The hydrogen isotopic data indicate that the source rocks are formed in terrestrial limnetic facies with freshwater. Natural gases from Well Ba23 and Well Ke19 experienced biodegradation in the late stage.
Turpan-Hami Basin is a major petroliferous basin in China. To date the natural gas exploration is concentrated in the Taibei sag. The origin and source of natural gas in the Taibei sag has long been controversial. To further investigate the origin and source of the natural gas in the Taibei sag, combined with previous studies and the local geological backgrounds, this study collected 23 gas samples from the Baka, Qiuling, Shanshan and Wenmi oil fields in the Taibei sag and analyzed the sample composition, stable carbon and hydrogen isotopes of all the gas samples. The results show that, gases from the four oil fields in the Taibei sag are dominated by hydrocarbon gas and belong to wet gas. Methane accounts for 65.84% to 97.94%, the content of heavy hydrocarbon(C2-5) can be up to 34.98%, while the content of nonhydrocarbon(CO_2, N_2) is trace. The δ~(13) C_1 value is –44.9‰ to –40.4‰, δ~(13) C_2 is –28.2‰ to –24.9‰, δ~(13) C_3 is –27.1‰ to–18.0‰ and δ~(13) C_4 is –26.7‰ to –22.1; while the variation of δD1 is not significant from –272‰ to –252‰, δD_2 is –236‰ to –200‰ and δD_3 is –222‰ to –174‰. Methane and its homologues(C_(2-5)) are characterized by normal stable carbon and hydrogen isotopic distribution pattern, i.e., with the increase of carbon number, methane and its homologues become more and more enriched in 13 C or D(δ~(13) C_1<δ~(13) C_2<δ~(13) C_3<δ~(13) C_4<δ~(13) C_5, δD1<δD_2<δD_3), which is consistent with the carbon and hydrogen isotopic features of typical thermogenic gas. All these results show that the natural gases in the four oil fields are coal-derived gas with low maturity(Ro averaged at0.7%), and are sourced from the Middle-Lower Jurassic coal measure. The hydrogen isotopic data of natural gas are affected by both thermal maturity and the water medium of the environment where source rocks are formed. The hydrogen isotopic data indicate that the source rocks are formed in terrestrial limnetic facies with freshwater. Natural gases from Well Ba23 and Well Ke19 experienced biodegradation in the late stage.
引文
[1]DAI Jinxing.Petroleum and natural gas generation during coalification.Petroleum Exploration and Development,1979,6(3):10-17.
[2]DAI Jinxing.Coal-derived gas theory and its discrimination.Chinese Science Bulletin,2018,63(14):1291-1305.
[3]NI Yunyan,ZHANG Dijia,LIAO Fengrong,et al.Stable hydrogen and carbon isotopic ratios of coal-derived gases from the Turpan-Hami Basin,NW China.International Journal of Coal Geology,2015,152(Part A):144-155.
[4]DAI Jinxing.Characteristics of carbon and hydrogen isotopes of natural gases and their discriminations.Natural Gas Geoscience,1993(2/3):1-40.
[5]WANG Wanchun.Geochemical characteristics of hydrogen isotopic compositions of natural gas,oil and kerogen.Acta Sedimentologic Sinica,1996,14(S1):131-135.
[6]LIU Quanyou,DAI Jinxing,LI Jian,et al.Hydrogen isotope composition of natural gases from the Tarim Basin and its indication of depositional environments of the source rocks.SCIENCE CHINA Earth Sciences,2008,51(2):300-311.
[7]SCHOELL M.The hydrogen and carbon isotopic composition of methane from natural gases of various origins.Geochimica et Cosmochimica Acta,1980,44(5):649-661.
[8]DAI Jinxing,NI Yunyan,ZOU Caineng.Stable carbon and hydrogen isotopes of natural gases sourced from the Xujiahe Formation in the Sichuan Basin,China.Organic Geochemistry,2012,43:103-111.
[9]SHEN Ping,XU Yongchang.The isotopic composition of natural gases from continental sediments in China.Geochimica,1991(2):144-152.
[10]WANG Xiaofeng,LIU Wenhui,SHI Baoguang,et al.Hydrogen isotope characteristics of thermogenic methane in Chinese sedimentary basins.Organic Geochemistry,2015,83/84:178-189.
[11]WANG Changgui,CHENG Keming,XU Yongchang,et al.Geochemistry of the Jurassic coal-derived hydrocarbon in the Turpan-Hami Basin.Beijing:Science Press,1998.
[12]SU Chuanguo,ZHU Jianguo,MENG Wangcai,et al.Discussion on generation mechanism of coal-formed oil in Turpan-Hami Basin.Tuha Oil&Gas,2005,10(1):14-20.
[13]CHEN Jianping,HUANG Difan,LI Jinchao,et al.Main source rocks of petroleum from Jurassic coal-bearing strata in the Turpan-Hami Basin,northwest China.Acta Geologica Sinica,1999,73(2):140-152.
[14]CHENG Keming.Oil and gas generation of the Turpan-Hami Basin.Beijing:Petroleum Industry Press,1994.
[15]WANG Yu,LI Jian,GUO Jianying,et al.Coal-fired gas identification and gas source analysis in Taipei Sag,Turpan-Hami Basin.Coal Technology,2018,37(10):148-150.
[16]XU Yongchang,WANG Zhiyong,WANG Xiaofeng,et al.Low-mature gases and typical low-mature gas fields in China.SCIENCE CHINA Earth Sciences,2008,51(2):312-320.
[17]LIU Bo,HUANG Zhilong,LUO Quansheng,et al.Accumulation mode and resource of lower Jurassic gas reservoir of Northern Foothill Belt,Turpan-Hami Basin.Journal of Central South University(Science and Technology Edition),2012,43(1):258-264.
[18]ZENG Fangang,WU Chaodong,SU Chuanguo.Genetic type of natural gas in Turpan-Hami Basin.Oil&Gas Geology,1998,19(2):76-78.
[19]GUO Xiaobo,WANG Haifu,HUANG Zhilong,et al.Geochemical analysis of tight sandstone gas in Qiudong subsag of Tuha Basin.Special Oil and Gas Reservoirs,2016,23(4):33-36.
[20]GAO Gang,LIANG Hao,LI Huaming,et al.Organic geochemistry of Carboniferous and Lower Permian source rocks,Turpan-Hami Basin,NW China.Petroleum Exploration and Development,2009,36(5):583-592.
[21]DAI Jinxing,XIA Xinyu,LI Zhisheng,et al.Inter-laboratory calibration of natural gas round robins for?2H and?13C using off-line and on-line techniques.Chemical Geology,2012,310/311:49-55.
[22]SHEN Ping,XU Yongchang,WANG Xianbin,et al.Geochemical characteristics of gas source rocks and natural gas genesis.Lanzhou:Gansu Science and Technology Press,1991.
[23]DAI Jinxing,QI Houfa.Relationship ofδ13C-Ro of coal-derived gas in China.Chinese Science Bulletin,1989,34(9):690-692.
[24]LIU Wenhui,XU Yongchang.A two-stage model of carbon isotopic fractionation in coal-gas.Geochimica,1999,28(4):359-366.
[25]DAI Jinxing,XIA Xinyu,QIN Shengfei,et al.Origins of partially reversed alkaneδ13C values for biogenic gases in China.Organic Geochemistry,2004,35(4):405-411.
[26]Des MARAIS D J,DONCHIN J H,NEHRING N L,et al.Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons.Nature,1981,292(5826):826-828.
[27]WHITICAR M J.Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane.Chemical Geology,1999,161(1):291-314.
[28]BERNARD B B,BROOKS J M,SACKETT W M.Natural gas seepage in the Gulf of Mexico.Earth and Planetary Science Letters,1976,31(1):48-54.
[29]DAI Jinxing,PEI Xigu,QI Houfa.Natural gas geology in China:Vol.1.Beijing:Petroleum Industry Press,1992.
[30]DAI Jinxing,QIN Shengfei,TAO Shizhen,et al.Developing trends of natural gas industry and the significant progress on natural gas geological theories in China.Natural Gas Geoscience,2005,16(2):127-142.
[31]XIAO Zhihua,XIE Zengye,LI Zhisheng,et al.Isotopic characteristics of natural gas of Xujiahe Formation in southern and middle of Sichuan Basin.Geochimica,2008,37(3):245-250.
[32]CHEN Jianfa,LI Chunyuan,SHEN Ping,et al.Carbon and hydrogen isotopic characteristics of hydrocarbons in coal type gas from China.Acta Sedimentologic Sinica,1995,13(2):59-69.
[33]WANG Shiqian,LUO Qihou,DENG Hongbin,et al.Characteristics of forming Jurassic gas reservoirs in the west part of Sichuan Basin.Natural Gas Industry,2001,21(2):1-8.
[34]GANG Wenzhe,GAO Gang,HAO Shisheng,et al.Carbon isotope of ethane applied in the analyses of genetic types of natural gas.Experimental Petroleum Geology,1997,19(2):164-167.
[35]TANG Y,PERRY J K,JENDEN P D,et al.Mathematical modeling of stable carbon isotope ratios in natural gases.Geochimica et Cosmochimica Acta,2000,64(15):2268-2673.
[36]JENDEN P D,NEWELL K D,KAPLAN I R,et al.Composition and stable-isotope geochemistry of natural gases from Kansas,Midcontinent,U.S.A.Chemical Geology,1988,71(1/2/3):117-147.
[37]BERNER U,FABER E.Empirical carbon isotope/maturity relationships for gases from algal kerogens and terrigenous organic matter,based on dry,open-system pyrolysis.Organic Geochemistry,1996,24(10/11):947-955.
[38]ROONEY M A,CLAYPOOL G E,CHUNG H M.Modeling thermogenic gas generation using carbon isotope ratios of natural gas hydrocarbons.Chemical Geology,1995,126(3/4):219-232.
[39]DAI Jinxing,NI Yunyan,WU Xiaoqi.Tight gas in China and its significance in exploration and exploitation.Petroleum Exploration and Development,2012,39(3):277-284.
[40]WANG Yaoping,ZOU Yanrong,ZHAN Zhaowen,et al.Origin of natural gas in the Turpan-Hami Basin,NW China:Evidence from pyrolytic simulation experiment.International Journal of Coal Geology,2018,195:238-249.
[41]GONG Deyu,MA Ruolong,GANG Chen,et al.Geochemical characteristics of biodegraded natural gas and its associated low molecular weight hydrocarbons.Journal of Natural Gas Science and Engineering,2017,46:338-349.
[42]STAHL W J,CAREY B D.Source-rock identification by isotope analyses of natural gases from fields in the Val Verde and Delaware basins,west Texas.Chemical Geology,1975,16(4):257-267.
[43]GALIMOV E M.Isotope organic geochemistry.Organic GeGeochemistry,2006,37(10):1126-1200.
[44]BIGELEISEN J.Chemistry of isotopes.Science,1965,147(3657):463-471.
[45]CRISS R E.Principles of stable isotope distribution.New York:Oxford University Press,1999.
[46]NI Y Y,MA Q SH,ELLIS G S,et al.Fundamental studies on kinetic isotope effect(KIE)of hydrogen isotope fractionation in natural gas systems.Geochimica et Cosmochimica Acta,2011,75(10):2270-2696.
[47]NI Yunyan,DAI Jinxing,ZHU Guangyou,et al.Stable hydrogen and carbon isotopic ratios of coal-derived and oil-derived gases:A case study in the Tarim basin,NW China.International Journal of Coal Geology,2013,116/117:302-313.
[48]TANG Y C,HUANG Y S,ELLIS G S,et al.A kinetic model for thermally induced hydrogen and carbon isotope fractionation of individual n-alkanes in crude oil.Geochimica et Cosmochimica Acta,2005,69(18):4452-4505.
[49]FENG Ziqi,DONG Dazhong,TIAN Jinqiang,et al.Geochemical characteristics of Longmaxi Formation shale gas in the Weiyuan area,Sichuan Basin,China.Journal of Petroleum Science and Engineering,2018,167:538-548.
[50]SHEN Ping,XU Yongchang.Isotopic compositional characteristics of terrigenous natural gases in China.Chinese Journal of Geochemistry,1993,12(1):14-24.
[51]SHEN Ping.Characteristics of carbon and hydrogen isotopic compositions of light hydrocarbons.SCIENTIA SINICAChimica,1995,38(2):211-220.
[52]WANG Zuodong,TAO Mingxin,MENG Qianxiang,et al.Research progress of source rocks and formation of low evolution oil and gas in Turpan-Hami Basin.Natural Gas Geoscience,2008,19(6):754-760.
[53]WANG Xiaofeng,LIU Wenhui,XU Yongchang,et al.Influences of water media on the hydrogen isotopic composition of natural gas/methane in the processes of gaseous hydrocarbon generation and evolution.SCIENCE CHINA Earth Sciences,2011,54(9):1318-1325.
[54]SESSIONS A L,SYLVA S P,SUMMONS R E,et al.Isotopic exchange of carbon-bound hydrogen over geologic timescales.Geochimica et Cosmochimica Acta Suppl.,2004,68(7):1545-1559.
[55]ALEXANDER R,KAGI R I,LARCHER A V.Clay catalysis of aromatic hydrogen-exchange reactions.Geochimica et Cosmochimica Acta,1982,46(2):219-222.
[56]SCHIMMELMANN A,LEWAN M D,WINTSCH R P.D/Hisotope ratios of kerogen,bitumen,oil,and water in hydrous pyrolysis of source rocks containing kerogen types I,II,IISand III.Geochimica et Cosmochimica Acta,1999,63(22):3751-3766.
[57]SCHIMMELMANN A,BOUDOU J P,LEWAN M D,et al.Experimental controls on D/H and 13C/12C ratios of kerogen,bitumen and oil during hydrous pyrolysis.Organic Geochemistry,2001,32(8):1009-1018.
[58]KINNAMAN F S,VALENTINE D L,TYLER S C.Carbon and hydrogen isotope fractionation associated with the aerobic microbial oxidation of methane,ethane,propane and butane.Geochimica et Cosmochimica Acta,2007,71(2):271-283.
[2]DAI Jinxing.Coal-derived gas theory and its discrimination.Chinese Science Bulletin,2018,63(14):1291-1305.
[3]NI Yunyan,ZHANG Dijia,LIAO Fengrong,et al.Stable hydrogen and carbon isotopic ratios of coal-derived gases from the Turpan-Hami Basin,NW China.International Journal of Coal Geology,2015,152(Part A):144-155.
[4]DAI Jinxing.Characteristics of carbon and hydrogen isotopes of natural gases and their discriminations.Natural Gas Geoscience,1993(2/3):1-40.
[5]WANG Wanchun.Geochemical characteristics of hydrogen isotopic compositions of natural gas,oil and kerogen.Acta Sedimentologic Sinica,1996,14(S1):131-135.
[6]LIU Quanyou,DAI Jinxing,LI Jian,et al.Hydrogen isotope composition of natural gases from the Tarim Basin and its indication of depositional environments of the source rocks.SCIENCE CHINA Earth Sciences,2008,51(2):300-311.
[7]SCHOELL M.The hydrogen and carbon isotopic composition of methane from natural gases of various origins.Geochimica et Cosmochimica Acta,1980,44(5):649-661.
[8]DAI Jinxing,NI Yunyan,ZOU Caineng.Stable carbon and hydrogen isotopes of natural gases sourced from the Xujiahe Formation in the Sichuan Basin,China.Organic Geochemistry,2012,43:103-111.
[9]SHEN Ping,XU Yongchang.The isotopic composition of natural gases from continental sediments in China.Geochimica,1991(2):144-152.
[10]WANG Xiaofeng,LIU Wenhui,SHI Baoguang,et al.Hydrogen isotope characteristics of thermogenic methane in Chinese sedimentary basins.Organic Geochemistry,2015,83/84:178-189.
[11]WANG Changgui,CHENG Keming,XU Yongchang,et al.Geochemistry of the Jurassic coal-derived hydrocarbon in the Turpan-Hami Basin.Beijing:Science Press,1998.
[12]SU Chuanguo,ZHU Jianguo,MENG Wangcai,et al.Discussion on generation mechanism of coal-formed oil in Turpan-Hami Basin.Tuha Oil&Gas,2005,10(1):14-20.
[13]CHEN Jianping,HUANG Difan,LI Jinchao,et al.Main source rocks of petroleum from Jurassic coal-bearing strata in the Turpan-Hami Basin,northwest China.Acta Geologica Sinica,1999,73(2):140-152.
[14]CHENG Keming.Oil and gas generation of the Turpan-Hami Basin.Beijing:Petroleum Industry Press,1994.
[15]WANG Yu,LI Jian,GUO Jianying,et al.Coal-fired gas identification and gas source analysis in Taipei Sag,Turpan-Hami Basin.Coal Technology,2018,37(10):148-150.
[16]XU Yongchang,WANG Zhiyong,WANG Xiaofeng,et al.Low-mature gases and typical low-mature gas fields in China.SCIENCE CHINA Earth Sciences,2008,51(2):312-320.
[17]LIU Bo,HUANG Zhilong,LUO Quansheng,et al.Accumulation mode and resource of lower Jurassic gas reservoir of Northern Foothill Belt,Turpan-Hami Basin.Journal of Central South University(Science and Technology Edition),2012,43(1):258-264.
[18]ZENG Fangang,WU Chaodong,SU Chuanguo.Genetic type of natural gas in Turpan-Hami Basin.Oil&Gas Geology,1998,19(2):76-78.
[19]GUO Xiaobo,WANG Haifu,HUANG Zhilong,et al.Geochemical analysis of tight sandstone gas in Qiudong subsag of Tuha Basin.Special Oil and Gas Reservoirs,2016,23(4):33-36.
[20]GAO Gang,LIANG Hao,LI Huaming,et al.Organic geochemistry of Carboniferous and Lower Permian source rocks,Turpan-Hami Basin,NW China.Petroleum Exploration and Development,2009,36(5):583-592.
[21]DAI Jinxing,XIA Xinyu,LI Zhisheng,et al.Inter-laboratory calibration of natural gas round robins for?2H and?13C using off-line and on-line techniques.Chemical Geology,2012,310/311:49-55.
[22]SHEN Ping,XU Yongchang,WANG Xianbin,et al.Geochemical characteristics of gas source rocks and natural gas genesis.Lanzhou:Gansu Science and Technology Press,1991.
[23]DAI Jinxing,QI Houfa.Relationship ofδ13C-Ro of coal-derived gas in China.Chinese Science Bulletin,1989,34(9):690-692.
[24]LIU Wenhui,XU Yongchang.A two-stage model of carbon isotopic fractionation in coal-gas.Geochimica,1999,28(4):359-366.
[25]DAI Jinxing,XIA Xinyu,QIN Shengfei,et al.Origins of partially reversed alkaneδ13C values for biogenic gases in China.Organic Geochemistry,2004,35(4):405-411.
[26]Des MARAIS D J,DONCHIN J H,NEHRING N L,et al.Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons.Nature,1981,292(5826):826-828.
[27]WHITICAR M J.Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane.Chemical Geology,1999,161(1):291-314.
[28]BERNARD B B,BROOKS J M,SACKETT W M.Natural gas seepage in the Gulf of Mexico.Earth and Planetary Science Letters,1976,31(1):48-54.
[29]DAI Jinxing,PEI Xigu,QI Houfa.Natural gas geology in China:Vol.1.Beijing:Petroleum Industry Press,1992.
[30]DAI Jinxing,QIN Shengfei,TAO Shizhen,et al.Developing trends of natural gas industry and the significant progress on natural gas geological theories in China.Natural Gas Geoscience,2005,16(2):127-142.
[31]XIAO Zhihua,XIE Zengye,LI Zhisheng,et al.Isotopic characteristics of natural gas of Xujiahe Formation in southern and middle of Sichuan Basin.Geochimica,2008,37(3):245-250.
[32]CHEN Jianfa,LI Chunyuan,SHEN Ping,et al.Carbon and hydrogen isotopic characteristics of hydrocarbons in coal type gas from China.Acta Sedimentologic Sinica,1995,13(2):59-69.
[33]WANG Shiqian,LUO Qihou,DENG Hongbin,et al.Characteristics of forming Jurassic gas reservoirs in the west part of Sichuan Basin.Natural Gas Industry,2001,21(2):1-8.
[34]GANG Wenzhe,GAO Gang,HAO Shisheng,et al.Carbon isotope of ethane applied in the analyses of genetic types of natural gas.Experimental Petroleum Geology,1997,19(2):164-167.
[35]TANG Y,PERRY J K,JENDEN P D,et al.Mathematical modeling of stable carbon isotope ratios in natural gases.Geochimica et Cosmochimica Acta,2000,64(15):2268-2673.
[36]JENDEN P D,NEWELL K D,KAPLAN I R,et al.Composition and stable-isotope geochemistry of natural gases from Kansas,Midcontinent,U.S.A.Chemical Geology,1988,71(1/2/3):117-147.
[37]BERNER U,FABER E.Empirical carbon isotope/maturity relationships for gases from algal kerogens and terrigenous organic matter,based on dry,open-system pyrolysis.Organic Geochemistry,1996,24(10/11):947-955.
[38]ROONEY M A,CLAYPOOL G E,CHUNG H M.Modeling thermogenic gas generation using carbon isotope ratios of natural gas hydrocarbons.Chemical Geology,1995,126(3/4):219-232.
[39]DAI Jinxing,NI Yunyan,WU Xiaoqi.Tight gas in China and its significance in exploration and exploitation.Petroleum Exploration and Development,2012,39(3):277-284.
[40]WANG Yaoping,ZOU Yanrong,ZHAN Zhaowen,et al.Origin of natural gas in the Turpan-Hami Basin,NW China:Evidence from pyrolytic simulation experiment.International Journal of Coal Geology,2018,195:238-249.
[41]GONG Deyu,MA Ruolong,GANG Chen,et al.Geochemical characteristics of biodegraded natural gas and its associated low molecular weight hydrocarbons.Journal of Natural Gas Science and Engineering,2017,46:338-349.
[42]STAHL W J,CAREY B D.Source-rock identification by isotope analyses of natural gases from fields in the Val Verde and Delaware basins,west Texas.Chemical Geology,1975,16(4):257-267.
[43]GALIMOV E M.Isotope organic geochemistry.Organic GeGeochemistry,2006,37(10):1126-1200.
[44]BIGELEISEN J.Chemistry of isotopes.Science,1965,147(3657):463-471.
[45]CRISS R E.Principles of stable isotope distribution.New York:Oxford University Press,1999.
[46]NI Y Y,MA Q SH,ELLIS G S,et al.Fundamental studies on kinetic isotope effect(KIE)of hydrogen isotope fractionation in natural gas systems.Geochimica et Cosmochimica Acta,2011,75(10):2270-2696.
[47]NI Yunyan,DAI Jinxing,ZHU Guangyou,et al.Stable hydrogen and carbon isotopic ratios of coal-derived and oil-derived gases:A case study in the Tarim basin,NW China.International Journal of Coal Geology,2013,116/117:302-313.
[48]TANG Y C,HUANG Y S,ELLIS G S,et al.A kinetic model for thermally induced hydrogen and carbon isotope fractionation of individual n-alkanes in crude oil.Geochimica et Cosmochimica Acta,2005,69(18):4452-4505.
[49]FENG Ziqi,DONG Dazhong,TIAN Jinqiang,et al.Geochemical characteristics of Longmaxi Formation shale gas in the Weiyuan area,Sichuan Basin,China.Journal of Petroleum Science and Engineering,2018,167:538-548.
[50]SHEN Ping,XU Yongchang.Isotopic compositional characteristics of terrigenous natural gases in China.Chinese Journal of Geochemistry,1993,12(1):14-24.
[51]SHEN Ping.Characteristics of carbon and hydrogen isotopic compositions of light hydrocarbons.SCIENTIA SINICAChimica,1995,38(2):211-220.
[52]WANG Zuodong,TAO Mingxin,MENG Qianxiang,et al.Research progress of source rocks and formation of low evolution oil and gas in Turpan-Hami Basin.Natural Gas Geoscience,2008,19(6):754-760.
[53]WANG Xiaofeng,LIU Wenhui,XU Yongchang,et al.Influences of water media on the hydrogen isotopic composition of natural gas/methane in the processes of gaseous hydrocarbon generation and evolution.SCIENCE CHINA Earth Sciences,2011,54(9):1318-1325.
[54]SESSIONS A L,SYLVA S P,SUMMONS R E,et al.Isotopic exchange of carbon-bound hydrogen over geologic timescales.Geochimica et Cosmochimica Acta Suppl.,2004,68(7):1545-1559.
[55]ALEXANDER R,KAGI R I,LARCHER A V.Clay catalysis of aromatic hydrogen-exchange reactions.Geochimica et Cosmochimica Acta,1982,46(2):219-222.
[56]SCHIMMELMANN A,LEWAN M D,WINTSCH R P.D/Hisotope ratios of kerogen,bitumen,oil,and water in hydrous pyrolysis of source rocks containing kerogen types I,II,IISand III.Geochimica et Cosmochimica Acta,1999,63(22):3751-3766.
[57]SCHIMMELMANN A,BOUDOU J P,LEWAN M D,et al.Experimental controls on D/H and 13C/12C ratios of kerogen,bitumen and oil during hydrous pyrolysis.Organic Geochemistry,2001,32(8):1009-1018.
[58]KINNAMAN F S,VALENTINE D L,TYLER S C.Carbon and hydrogen isotope fractionation associated with the aerobic microbial oxidation of methane,ethane,propane and butane.Geochimica et Cosmochimica Acta,2007,71(2):271-283.