生物降解稠油沥青质热解产物中生物标志化合物与单体烃碳同位素组成研究
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摘要
本文运用热解技术对采自准噶尔盆地风城地区6个重度生物降解稠油进行沥青质热解实验。通过分析沥青质热解产物中生物标志化合物组成和单体正构烷烃碳同位素组成,探索其在降解稠油油源研究中的应用。研究结果显示,沥青质热解产物中生物标志化合物组成特征易受热解温度的影响,指示母质沉积水体环境的参数Pr/Ph比值随热解温度升高逐渐增大,在较高的温度下,高碳数、高环数的生物标志化合物易裂解生成低碳数、低环数的化合物,导致C_(20)三环萜烷/C_(30)藿烷和孕甾烷/αααC_(29)R甾烷两个参数的比值随热解温度升高逐渐增大,表明利用沥青质热解产物生物标志化合物组成进行降解稠油油源判识易出现偏差。而沥青质热解产物单体正构烷烃碳同位素组成随热解温度升高并没有明显的变化,6个降解稠油沥青质热解产物单体正构烷烃碳同位素分布曲线呈水平分布,与来自风城组烃源岩的典型原油基本相似,说明沥青质热解产物中单体烃碳同位素组成特征可用于重度降解稠油油源分析。另外,通过对比稠油与其沥青质热解产物中单体正构烷烃单体碳同位素组成差异,可用于研究多油源以及后期混入的问题。
This research performed pyrolysis on the asphaltenes of six biodegraded heavy oils from the Fengcheng area of the Junggar Basin to investigate the biomarker and carbon isotopic compositions of individual n-alkanes in the asphaltene pyrolysis products and their application in the study of biodegaraeded oil source correlations.The results showed that the biomarker composition in the asphaltene pyrolysis products was susceptible to the pyrolysis temperature.The Pr/Ph value which indicates the sedimentary water environment,increases with the rise of pyrolysis temperature.The high carbon number and high ring number biomarkers,which made the C_(20) tricyclic terpane/C_(30) hopane value and the pregnant sterane/αααC_(29)R sterane value increase with the pyrolysis temperature increase.Using the biomarker composition of the asphaltene pyrolysis products in a biodegraded heavy oil source correlation study will produce a deviation.No significant change in the carbon isotopic composition of individua n-alkanes in the asphaltene pyrolysis products was observed with the pyrolysis temperature increase.Moreover the distribution curves of the carbon isotopes of the n-alkanes in the asphaltene pyrolysis products from six biodegraded heavy oils were in a horizontal position similar to the typical crude oil from the source rocks of the Fengcheng formation.The carbon isotopic composition of individual n-alkanes in the asphaltene pyrolysis products can be used for the biodegraded heavy oil source correlation study.A comparison of the carbon isotopic composition of the n-alkanes in the biodegraded heavy oil and its asphaltene pyrolysis products can also be used to study the differentiated varieties of oil source and input.
This research performed pyrolysis on the asphaltenes of six biodegraded heavy oils from the Fengcheng area of the Junggar Basin to investigate the biomarker and carbon isotopic compositions of individual n-alkanes in the asphaltene pyrolysis products and their application in the study of biodegaraeded oil source correlations.The results showed that the biomarker composition in the asphaltene pyrolysis products was susceptible to the pyrolysis temperature.The Pr/Ph value which indicates the sedimentary water environment,increases with the rise of pyrolysis temperature.The high carbon number and high ring number biomarkers,which made the C_(20) tricyclic terpane/C_(30) hopane value and the pregnant sterane/αααC_(29)R sterane value increase with the pyrolysis temperature increase.Using the biomarker composition of the asphaltene pyrolysis products in a biodegraded heavy oil source correlation study will produce a deviation.No significant change in the carbon isotopic composition of individua n-alkanes in the asphaltene pyrolysis products was observed with the pyrolysis temperature increase.Moreover the distribution curves of the carbon isotopes of the n-alkanes in the asphaltene pyrolysis products from six biodegraded heavy oils were in a horizontal position similar to the typical crude oil from the source rocks of the Fengcheng formation.The carbon isotopic composition of individual n-alkanes in the asphaltene pyrolysis products can be used for the biodegraded heavy oil source correlation study.A comparison of the carbon isotopic composition of the n-alkanes in the biodegraded heavy oil and its asphaltene pyrolysis products can also be used to study the differentiated varieties of oil source and input.
引文
[1]Tissot B P,Welte D H.Petroleum Formation and Occurrence[M].NewYork:Springer-Verlag,1984:1-699.
[2]Roadifer R E.Size Distribution of World’s Largest Known Oil and Tar Accumulation[M].Tulsa:AAPG Studies in Geology,1987:3-23.
[3]Head I M,Jones D M,Larter S R.Biological activity in the deep subsurface and the origin of heavy oil[J].Nature,2003,426(6964):344-352.
[4]韩霞,吴拓,徐冠军,李培新,马玉东.生物降解稠油油源对比新方法及其应用[J].特种油气藏,2007,14(5):98-101.Han Xia,Wu Tuo,Xu Guan-jun,Li Pei-xin,Ma Yu-dong.Anew method of oil and source rock correlation and its application in biodegradation heavy oil[J].Spec Oil Gas Reser,2007,14(5):98-101(in Chinese with English abstract).
[5]朱军,李术元,郭绍辉.生物降解原油研究的新方法[J].燃料化学学报,2003,31(1):1-4.Zhu Jun,Li Shu-yuan,Guo Shao-hui.New methods for the study of biodegraded crude oil[J].J Fuel Chem Tech,2003,31(1):1-4(in Chinese with English abstract).
[6]Sofer Z.Hydrous pyrolysis of montoerey asphaltenes[J].Org Geochem,1988,13(4-6):939-945.
[7]Rubinstein I,Spyckerelle C,Strausz O P.Pyrolysis of asphaltenes:A source of geochemical information[J].Geochim Cosmochim Acta,1979,43(1):1-6.
[8]Des Marais D J,Donchin J H,Nehring N L,Truesdell A H.Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons[J].Nature,1981,292(5826):826-828.
[9]Laughrey C D,Baldassare F J.Geochemistry and origin of some natural gases in the Plateau Province,Central Appalachian Basin[J].Am Assoc Pet Geol Bull,1998,82:317-335.
[10]由伟丰,孟闲龙.准噶尔盆地车排子地区排2井油源分析[J].中国西部油气地质,2006,2(1):56-59.You Wei-feng,Meng Xian-long.Oil source analysis of well P-2 in the Chepaizi area of the Junggar Basin[J].West China Pet Geosci,2006,2(1):56-59(in Chinese with English abstract).
[11]梁全胜,刘震,党玉琪.柴达木盆地三湖地区第四系生物气成因类型的研究[J].中国西部油气地质,2005,1(1):66-69.Liang Quan-sheng,Liu Zhen,Dang Yu-qi.Quaternary biogenic gas cause types in the Sanhu region of the eastern Qaidam Basin[J].West China Pet Geosci,2005,1(1):66-69(in Chinese with English abstract).
[12]Freeman K H,Hayes J M,Trendel J M,Albrecht P.Evidence from carbon isotope measurements for diverse origins of sedimentary hydrocarbons[J].Nature,1990,343(6255):254-256.
[13]Collister J M,Summons R E,Lichtfouse E,Hayes J M.An isotopic biogeochemical study of the Green River oil shale[J].Org Geochem,1992,19(1-3):265-276.
[14]Hayes J M,Freeman K H,Popp B N,Hoham C H.Compound specific isotopic analyses:A novel tool for reconstruction of ancient biogeochemical processes[J].Org Geochem,1990,16(4-6):1115-1128.
[15]张文正,裴戈,关德师,程坤芳.中国几个盆地原油轻烃单体和正构烷烃系列分子碳同位素研究[J].地质论评,1993,39(1):79-85.Zhang Wen-zheng,Pei Ge,Guan De-shi,Cheng Kun-fang.The carbon isotopic composition of the light hydrocarbon monomer and normal alkane series molecules from crude oil of some petroliferous basins in China[J].Geol Rev,1993,39(1):79-85(in Chinese with English abstract).
[16]Simoneit B R T,Schoell M.Carbon isotope systematics of individual hydrocarbons in hydro thermal petroleums from the Guaymas Basin,Gulf of California[J].Org Geochem,1995,23(9):857-863.
[17]Bjoroy M,Hall P B,Mol R P.Variation in the isotopic composition of single components in the C4-C20 fraction of oils and condensates[J].Org Geochem,1994,21(6/7):761-776.
[18]Wilhelm S A,Larter S R,Hall K.A comparative study of the stable carbon isotopic composition of crude oil alkanes and associated crude oil asphaltene pyrolysate alkanes[J].Org Geochem,1994,21(6/7):751-759.
[19]王屿涛.准噶尔盆地西北缘稠油生物降解特征[J].沉积学报,1994,12(1):81-88.Wang Yu-tao.Characteristies of heavy oil biodegradation in the northwestern margin of Junggar basin[J].Acta Sediment Sinica,1994,12(1):81-88(in Chinese with English abstract).
[20]Peters K E,Moldowan J M.The Biomarker Guide:Interpreting Molecular Fossils in Petroleum and Ancient Sediments[M].Upper Saddle River:Prentice Hall Inc,1993:114-116.
[21]彭兴芳,李周波.生物标志化合物在石油地质中的应用[J].资源环境与工程,2006,20(3):279-283.Peng Xing-fang,Li Zhou-bo.The application of biomarker in the research of petroleum[J].Geo Res Environ Eng,2006,20(3):279-283(in Chinese with English abstract).
[22]王铁冠.生物标志物地球化学研究[M].武汉:中国地质大学出版社,1990:1-146.Wang Tie-guan.Study on Biomarkers Geochemistry[M].Wuhan:China University of Geosciences Press,1990:1-146(in Chinese).
[23]王绪龙,康素芳.准噶尔盆地腹部及西北缘斜坡区原油成因分析[J].新疆石油地质,1999,20(2):108-112.Wang Xu-long,Kang Su-fang.Analysis of crude origin in hinter land and slope of northwestern margin,Junggar basin[J].Xinjiang Pet Geol,1999,20(2):108-112(in Chinese with English abstract).
[24]高岗,向宝力,都鹏燕,马万云,陈哲龙,任江玲,柳广弟.准噶尔盆地玛湖凹陷风城组泥岩与泥质白云岩热模拟产物特征对比[J].地球科学与环境学报,2016,38(1):94-103.Gao Gang,Xiang Bao-li,Du Peng-yan,Ma Wan-yun,Chen Zhe-long,Ren Jiang-ling,Liu Guang-di.Comparison of thermal simulation product characteristics of mudstone and argillaceous dolomite from Fengcheng Formation in Mahu Sag of Junggar Basin[J].J Earth Sci Environ,2016,38(1):94-103.
[25]张立平,黄第藩,廖志勤.伽马蜡烷--水体分层的地球化学标志[J].沉积学报,1999,17(1):136-140.Zhang Li-ping,Huang Di-fan,Liao Zhi-qin.Gammaceranegeochemical indicator of water column stratification[J].Acta Sedimentol Sinica,1999,17(1):136-140(in Chinese with English abstract).
[26]黄攀,任江玲,李二庭,马万云,徐浩,于双,邹艳荣,潘长春.准噶尔盆地玛湖凹陷烃源岩和原油生物标志物与碳同位素组成及其意义[J].地球化学,2016,45(3):303-314.Huang Pan,Ren Jiang-ling,Li Er-ting,Ma Wan-yun,Xu Hao,Yu Shuang,Zou Yan-rong,Pan Chang-chun.Biomarker and carbon isotopic compositions of source rock extracts and crude oils from Mahu Sag,Junggar Basin[J].Geochimica,2016,45(3):303-314(in Chinese with English abstract).
[2]Roadifer R E.Size Distribution of World’s Largest Known Oil and Tar Accumulation[M].Tulsa:AAPG Studies in Geology,1987:3-23.
[3]Head I M,Jones D M,Larter S R.Biological activity in the deep subsurface and the origin of heavy oil[J].Nature,2003,426(6964):344-352.
[4]韩霞,吴拓,徐冠军,李培新,马玉东.生物降解稠油油源对比新方法及其应用[J].特种油气藏,2007,14(5):98-101.Han Xia,Wu Tuo,Xu Guan-jun,Li Pei-xin,Ma Yu-dong.Anew method of oil and source rock correlation and its application in biodegradation heavy oil[J].Spec Oil Gas Reser,2007,14(5):98-101(in Chinese with English abstract).
[5]朱军,李术元,郭绍辉.生物降解原油研究的新方法[J].燃料化学学报,2003,31(1):1-4.Zhu Jun,Li Shu-yuan,Guo Shao-hui.New methods for the study of biodegraded crude oil[J].J Fuel Chem Tech,2003,31(1):1-4(in Chinese with English abstract).
[6]Sofer Z.Hydrous pyrolysis of montoerey asphaltenes[J].Org Geochem,1988,13(4-6):939-945.
[7]Rubinstein I,Spyckerelle C,Strausz O P.Pyrolysis of asphaltenes:A source of geochemical information[J].Geochim Cosmochim Acta,1979,43(1):1-6.
[8]Des Marais D J,Donchin J H,Nehring N L,Truesdell A H.Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons[J].Nature,1981,292(5826):826-828.
[9]Laughrey C D,Baldassare F J.Geochemistry and origin of some natural gases in the Plateau Province,Central Appalachian Basin[J].Am Assoc Pet Geol Bull,1998,82:317-335.
[10]由伟丰,孟闲龙.准噶尔盆地车排子地区排2井油源分析[J].中国西部油气地质,2006,2(1):56-59.You Wei-feng,Meng Xian-long.Oil source analysis of well P-2 in the Chepaizi area of the Junggar Basin[J].West China Pet Geosci,2006,2(1):56-59(in Chinese with English abstract).
[11]梁全胜,刘震,党玉琪.柴达木盆地三湖地区第四系生物气成因类型的研究[J].中国西部油气地质,2005,1(1):66-69.Liang Quan-sheng,Liu Zhen,Dang Yu-qi.Quaternary biogenic gas cause types in the Sanhu region of the eastern Qaidam Basin[J].West China Pet Geosci,2005,1(1):66-69(in Chinese with English abstract).
[12]Freeman K H,Hayes J M,Trendel J M,Albrecht P.Evidence from carbon isotope measurements for diverse origins of sedimentary hydrocarbons[J].Nature,1990,343(6255):254-256.
[13]Collister J M,Summons R E,Lichtfouse E,Hayes J M.An isotopic biogeochemical study of the Green River oil shale[J].Org Geochem,1992,19(1-3):265-276.
[14]Hayes J M,Freeman K H,Popp B N,Hoham C H.Compound specific isotopic analyses:A novel tool for reconstruction of ancient biogeochemical processes[J].Org Geochem,1990,16(4-6):1115-1128.
[15]张文正,裴戈,关德师,程坤芳.中国几个盆地原油轻烃单体和正构烷烃系列分子碳同位素研究[J].地质论评,1993,39(1):79-85.Zhang Wen-zheng,Pei Ge,Guan De-shi,Cheng Kun-fang.The carbon isotopic composition of the light hydrocarbon monomer and normal alkane series molecules from crude oil of some petroliferous basins in China[J].Geol Rev,1993,39(1):79-85(in Chinese with English abstract).
[16]Simoneit B R T,Schoell M.Carbon isotope systematics of individual hydrocarbons in hydro thermal petroleums from the Guaymas Basin,Gulf of California[J].Org Geochem,1995,23(9):857-863.
[17]Bjoroy M,Hall P B,Mol R P.Variation in the isotopic composition of single components in the C4-C20 fraction of oils and condensates[J].Org Geochem,1994,21(6/7):761-776.
[18]Wilhelm S A,Larter S R,Hall K.A comparative study of the stable carbon isotopic composition of crude oil alkanes and associated crude oil asphaltene pyrolysate alkanes[J].Org Geochem,1994,21(6/7):751-759.
[19]王屿涛.准噶尔盆地西北缘稠油生物降解特征[J].沉积学报,1994,12(1):81-88.Wang Yu-tao.Characteristies of heavy oil biodegradation in the northwestern margin of Junggar basin[J].Acta Sediment Sinica,1994,12(1):81-88(in Chinese with English abstract).
[20]Peters K E,Moldowan J M.The Biomarker Guide:Interpreting Molecular Fossils in Petroleum and Ancient Sediments[M].Upper Saddle River:Prentice Hall Inc,1993:114-116.
[21]彭兴芳,李周波.生物标志化合物在石油地质中的应用[J].资源环境与工程,2006,20(3):279-283.Peng Xing-fang,Li Zhou-bo.The application of biomarker in the research of petroleum[J].Geo Res Environ Eng,2006,20(3):279-283(in Chinese with English abstract).
[22]王铁冠.生物标志物地球化学研究[M].武汉:中国地质大学出版社,1990:1-146.Wang Tie-guan.Study on Biomarkers Geochemistry[M].Wuhan:China University of Geosciences Press,1990:1-146(in Chinese).
[23]王绪龙,康素芳.准噶尔盆地腹部及西北缘斜坡区原油成因分析[J].新疆石油地质,1999,20(2):108-112.Wang Xu-long,Kang Su-fang.Analysis of crude origin in hinter land and slope of northwestern margin,Junggar basin[J].Xinjiang Pet Geol,1999,20(2):108-112(in Chinese with English abstract).
[24]高岗,向宝力,都鹏燕,马万云,陈哲龙,任江玲,柳广弟.准噶尔盆地玛湖凹陷风城组泥岩与泥质白云岩热模拟产物特征对比[J].地球科学与环境学报,2016,38(1):94-103.Gao Gang,Xiang Bao-li,Du Peng-yan,Ma Wan-yun,Chen Zhe-long,Ren Jiang-ling,Liu Guang-di.Comparison of thermal simulation product characteristics of mudstone and argillaceous dolomite from Fengcheng Formation in Mahu Sag of Junggar Basin[J].J Earth Sci Environ,2016,38(1):94-103.
[25]张立平,黄第藩,廖志勤.伽马蜡烷--水体分层的地球化学标志[J].沉积学报,1999,17(1):136-140.Zhang Li-ping,Huang Di-fan,Liao Zhi-qin.Gammaceranegeochemical indicator of water column stratification[J].Acta Sedimentol Sinica,1999,17(1):136-140(in Chinese with English abstract).
[26]黄攀,任江玲,李二庭,马万云,徐浩,于双,邹艳荣,潘长春.准噶尔盆地玛湖凹陷烃源岩和原油生物标志物与碳同位素组成及其意义[J].地球化学,2016,45(3):303-314.Huang Pan,Ren Jiang-ling,Li Er-ting,Ma Wan-yun,Xu Hao,Yu Shuang,Zou Yan-rong,Pan Chang-chun.Biomarker and carbon isotopic compositions of source rock extracts and crude oils from Mahu Sag,Junggar Basin[J].Geochimica,2016,45(3):303-314(in Chinese with English abstract).
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