东北漠河盆地甲烷碳氢稳定同位素异常及形成机制
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摘要
东北漠河盆地是我国陆域多年冻土区天然气水合物聚集成藏及勘探的潜在区域。近几年,在漠河盆地实施天然气水合物钻探实验井和气源探井的过程中发现,该区甲烷碳、氢同位素δ~(13) CCH4、δDCH4值明显偏低,负向偏移特征明显:碳同位素δ~(13) C_(CH_4) 值多数小于-60‰,最低达-82.9‰;氢同位素δD_(CH_4) 值绝大多数低于-350‰,最低达-450‰。通常,埋深小于1 500m的范围,甲烷碳同位素δ13 C_(CH_4) 值随深度增大,氢同位素δD_(CH_4) 值随深度减小;深度大于1 500m,甲烷碳、氢同位素δ13C_(CH_4) 、δD_(CH_4) 值随深度同步增大。研究表明:漠河盆地的甲烷碳稳定同位素负向偏移,主要与甲烷的微生物成因有关;甲烷氢稳定同位素负向偏移,则是盆地所处较高纬度独特气候引起的地表水蒸发或大气冷凝降水过程的瑞利蒸馏和乙酸发酵的甲烷生成方式共同作用的结果。
The Mohe Basin in northeastern China possesses the potential for gas hydrate accumulation and exploration in the permafrost zone of China.During a recent investigation of wells used for gas hydrate testing and gas source exploration,we discovered significant negative shifts in stable carbon and hydrogen isotopes of methane in the Mohe Basin.The measured δ~(13) C_(CH_4) andδD_(CH_4) values commonly ranged from-60‰to-82.9‰ and from-350‰ to-450‰,respectively.We also observed that at burial depth of approximately less than 1500 m,δ~(13) C_(CH_4) value generally increased with depth,whereas δD_(CH_4) value decreased;however,both values increased synchronously with burial depth at greater than 1500 m.We believe that the negative shifts of stable carbon isotope are associated with the microbial origin of methane;whilst the negative shifts of stable hydrogen isotope are the results of a combined effect of Rayleigh distillation during the evaporation of surface water or atmospheric condensation process driven by basin's unique climate at higher latitude,and methane production through acetate fermentation.
The Mohe Basin in northeastern China possesses the potential for gas hydrate accumulation and exploration in the permafrost zone of China.During a recent investigation of wells used for gas hydrate testing and gas source exploration,we discovered significant negative shifts in stable carbon and hydrogen isotopes of methane in the Mohe Basin.The measured δ~(13) C_(CH_4) andδD_(CH_4) values commonly ranged from-60‰to-82.9‰ and from-350‰ to-450‰,respectively.We also observed that at burial depth of approximately less than 1500 m,δ~(13) C_(CH_4) value generally increased with depth,whereas δD_(CH_4) value decreased;however,both values increased synchronously with burial depth at greater than 1500 m.We believe that the negative shifts of stable carbon isotope are associated with the microbial origin of methane;whilst the negative shifts of stable hydrogen isotope are the results of a combined effect of Rayleigh distillation during the evaporation of surface water or atmospheric condensation process driven by basin's unique climate at higher latitude,and methane production through acetate fermentation.
引文
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[25] WHITICAR M J,FABER E,SCHOELL M.Biogenic methane formation in marine and freshwater environments:CO2reduction vs.acetate fermentation-isotope evidence[J].Geochimica et Cosmochimica Acta,1986,50:693-709.
[26] MARTENS C S,BLAIR N E,GREEN C D,et al.Seasonal variations in the stable carbon isotopic signature of biogenic methane in a coastal sediment[J].Science,1986,233:1300-1303.
[27] BURKE R A,MARTENS C S,SACKETT W M.Seasonal variations of D/H and 13C/12C ratios of biogenic methane in surface sediment of Cape Lookout Bight,USA[J].Nature,1988,322:829-831.
[28] EDARD R C H,FREDRICK J L,WILLIAM S F.Spatial distribution of microbial methane production pathways in temperate zone wetland soils:stable carbon and hydrogen isotope evidence[J].Geochimica et Cosmochimica Acta,1997,61(44):745-753.
[2]张顺,林春明,吴朝东,等.黑龙江漠河盆地构造特征与成盆演化[J].高校地质学报,2003,9(3):411-418.
[3]吴根耀,冯志强,杨建国,等.中国东北漠河盆地的构造背景和地质演化[J].石油与天然气地质,2006,27(4):528-535.
[4] TISSOT B P,WELTA D H.Petroleum formation and occurrence[M].2nd ed.Berlin:Springer-Verlag,1984:1-699.
[5] XU S,NAKAI S,WAKITA H,et al.Carbon isotopes of hydrocarbons and carbon dioxide in natural gases in China[J].Journal of Asian Earth Sciences,1997,15(1):89-101.
[6] ZHANG S,HUANG H,FENG Z,et al.Geochemical characterization of secondary microbial gas occurrence in the Songliao Basin,NE China[J].Organic Geochemistry,2011,42:781-790.
[7] ZHU G,WANG Z,DAI J,et al.Natural gas constituent and carbon isotopic composition in petroliferous basins,China[J].Journal of Asian Earth Sciences,2014,80:1-17.
[8]戴金星,陈英.中国生物气中烷烃组分的碳同位素特征及其鉴别标志[J].中国科学:B辑,1993,23(3):303-310.
[9]沈平,王晓锋,徐茵,等.我国生物气藏碳、氢同位素特征、形成途径及意义[J].沉积学报,2010,28(1):183-187.
[10] RICE D D,CLAPOOL G E.Generation,accumulation,and resource potential of biogenic gas[J].AAPG Bulletin,1981,65(1):5-25.
[11] RICE D D.Composition and origin of coalbed gas[J].AAPG Studies in Geology,1993,38:159-183.
[12] WHITICAR M J.Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane[J].Chemical Geology,1999,161:291-314.
[13] NAKAGAWA F,YOSHIDA N.Production of methane from alasses in eastern Siberia:implications from its 14C and stable isotope compositions[J].Global Biogeochemical Cycles,2002,16(3):1041:14-1-14-5.
[14] SCHOELL M.Multiple origins of methane in the Earth[J].Chemical Geology,1988,71:1-10.
[15]赵省民,邓坚,饶竹,等.漠河盆地浅部气体特征及对天然气水合物形成的意义[J].石油学报,2018,39(3):266-277.
[16] SCHOELL l M.The hydrogen and carbon isotopic composition of methane from natural gases of various origins[J].Geochimica et Cosmochimica Acta,1980,44:649-661.
[17] INGRAHAM N L,TAYLOR B E.Hydrogen isotope study of large-scale meteoric water transport in northern California and Nevada[J].Journal of Hydrology,1986,85:183-197.
[18] KRISHNAN S,PAGANI M,HUBER M,et al.High latitude hydrological changes during the Eocene Thermal Maxmium2[J].Earth and Planetary Sciences Letters,2014,404:167-177.
[19] TIMISIC S,PATTERSON W P.Spatial variability in stable isotope values of surface waters of Eastern Canada and New England[J].Journal of Hydrology,2014,511:594-604.
[20] MARTENS C S,KELLEY C A,CHANTON J F.Carbon and hydrogen isotopic characterization of methane from wetlands and lakes of the Yukon-Kuskokwim delta,Western Alaska[J].Journal of Geophysical Research,1992,97(D15):16689-16701.
[21] CHANTON J P,FIELDS D,HINES M E.Controls on the hydrogen isotopic composition of biogenic methane from high-latitude terrestrial wetlands[J].Journal of Geophysical Research,2006,111(G04004):1-9.
[22] BELLISARIO L M,BUBIER J L,MOOR T R,et al.Controls on CH4emissions from a northern peatland[J].Global Biogeochemical Cycles,1999,13:81-91.
[23] SUGIMUTO A,WADA E.Hydrogen isotopic composition of bacterial methane:CO2/H2 reduction and acetate fermentation[J].Geochimica et Cosmochimica Acta,1995,59:1329-1337.
[24] MARTINI A M,WALTER L M,KU T C W,et al.Microbial production and modification of gases in sedimentary basins:ageochemical case study from a Devonian shale gas play,Michigan basin[J].AAPG Bulletin,2003,87:1355-1375.
[25] WHITICAR M J,FABER E,SCHOELL M.Biogenic methane formation in marine and freshwater environments:CO2reduction vs.acetate fermentation-isotope evidence[J].Geochimica et Cosmochimica Acta,1986,50:693-709.
[26] MARTENS C S,BLAIR N E,GREEN C D,et al.Seasonal variations in the stable carbon isotopic signature of biogenic methane in a coastal sediment[J].Science,1986,233:1300-1303.
[27] BURKE R A,MARTENS C S,SACKETT W M.Seasonal variations of D/H and 13C/12C ratios of biogenic methane in surface sediment of Cape Lookout Bight,USA[J].Nature,1988,322:829-831.
[28] EDARD R C H,FREDRICK J L,WILLIAM S F.Spatial distribution of microbial methane production pathways in temperate zone wetland soils:stable carbon and hydrogen isotope evidence[J].Geochimica et Cosmochimica Acta,1997,61(44):745-753.
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