淡水和咸水湖相泥质烃源岩不同赋存态有机质的地球化学特征
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摘要
泥质烃源岩中的有机质存在多种赋存形式,其中与无机矿物结合形成有机—无机复合体是有机质保存的重要方式之一。为了对比研究泥质烃源岩中不同赋存态有机质的地球化学特征,选取东营凹陷沙三下亚段(淡水湖相)和沙四上亚段(咸水湖相)优质烃源岩为研究对象,采用"溶剂抽提—皂化—HCl酸解—HF/HCl酸解"的连续处理实验方法,依次得到烃源岩中的游离态有机质、黏土矿物层间吸附有机质、碳酸盐矿物结合有机质和黏土矿物表面化学吸附有机质。结果表明,烃源岩中的矿物结合态有机质约占可溶有机质总量的10%,矿物结合态有机质与游离态有机质表现出显著的地化特征差异:矿物结合态有机质以非烃、沥青质等极性组分为主要组成,饱和烃中轻烃比例较高;矿物结合态有机质可以补充保存具有生源指示意义的分子标志物,如指示Botryococcus braunii生源的两环倍半萜类分子标志物仅在碳酸盐矿物结合有机质中检出,指示古菌生源的角鲨烷仅在HF/HCl酸解有机质中检出;此外,矿物结合态有机质亦可对沉积环境的差异做出分子响应。因此,在对游离态有机质地化特征分析基础上,如能综合分析不同矿物结合态有机质的地化特征,可以获得更为全面的地质分析结果。
Organic matter( OM) in argillaceous source rocks occurs in various forms,and it is common for OM be bounded to minerals forming OM-mineral complexes. In order to geochemically characterize OM of different occurrences,some high quality source rocks were sampled from the lower third member( Es3) and the upper fourth member( Es4) of the Shahejie Formation in the Dongying Sag,and were subjected to sequential treatments as follows: solvent extraction-saponification-hydrochloric acid hydrolysis-hydrofluoric acid hydrolysis. The free,clay interlayer absorbed,carbonate-bound,and clay surface-bound OM were successively released and GC-MS analyzed.Results indicated that the mineral-bound OM accounted for approximately 10% of the total soluble OM in source rocks,and there exists distinct geochemical differences between the free and mineral-bound OM,with the latter dominated by polar fractions such as nonhydrocarbons and asphaltene. The former comprised higher proportions of light hydrocarbons,and selectively preserved biomarkers indicative of biogenic origin,like the bicyclic sesquiterpenoids in the carbonate-bound OM,indicative of input from Botryococcus braunii,and squalane in the clay surface-bound OM,indicative of input from archaea. The mineral-bound OM was also sensitive to environmental changes,and exhibited molecular differences between fresh Es3 and saline Es4 samples. Thus,it was concluded that comprehensive geochemical investigation of the free and mineral-bound OM in argillaceous source rocks could achieve more authentic geological interpretations. Besides,molecular characterization of hydrocarbons of various occurrences could help further elucidate OM preservation mechanisms,as well as better evaluate source rock potential.
Organic matter( OM) in argillaceous source rocks occurs in various forms,and it is common for OM be bounded to minerals forming OM-mineral complexes. In order to geochemically characterize OM of different occurrences,some high quality source rocks were sampled from the lower third member( Es3) and the upper fourth member( Es4) of the Shahejie Formation in the Dongying Sag,and were subjected to sequential treatments as follows: solvent extraction-saponification-hydrochloric acid hydrolysis-hydrofluoric acid hydrolysis. The free,clay interlayer absorbed,carbonate-bound,and clay surface-bound OM were successively released and GC-MS analyzed.Results indicated that the mineral-bound OM accounted for approximately 10% of the total soluble OM in source rocks,and there exists distinct geochemical differences between the free and mineral-bound OM,with the latter dominated by polar fractions such as nonhydrocarbons and asphaltene. The former comprised higher proportions of light hydrocarbons,and selectively preserved biomarkers indicative of biogenic origin,like the bicyclic sesquiterpenoids in the carbonate-bound OM,indicative of input from Botryococcus braunii,and squalane in the clay surface-bound OM,indicative of input from archaea. The mineral-bound OM was also sensitive to environmental changes,and exhibited molecular differences between fresh Es3 and saline Es4 samples. Thus,it was concluded that comprehensive geochemical investigation of the free and mineral-bound OM in argillaceous source rocks could achieve more authentic geological interpretations. Besides,molecular characterization of hydrocarbons of various occurrences could help further elucidate OM preservation mechanisms,as well as better evaluate source rock potential.
引文
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[4]杨燕,雷天柱,邢蓝田,等.不同类型有机黏土中化学结合态有机质生油能力差异性研究[J].石油实验地质,2015,37(4):487-493.YANG Yan,LEI Tianzhu,XING Lantian,et al. Oil generation abilities of chemically bound organic matter in different types of organic clay complexes[J]. Petroleum Geology&Experiment,2015,37(4):487-493.
[5]蔡进功,宋明水,卢龙飞,等.烃源岩中有机黏粒复合体:天然的生烃母质[J].海洋地质与第四纪地质,2013,33(3):123-131.CAI Jingong,SONG Mingshui,LU Longfei,et al.Organo-clay complexes in source rocks:a natural material for hydrocarbon generation[J].Marine Geology&Quaternary Geology,2013,33(3):123-131.
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[7] KENNEDY M J,PEVEAR D R,HILL R J.Mineral surface control of organic carbon in black shale[J].Science,2002,295(5555):657-660.
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[9]蒋启贵,黎茂稳,钱门辉,等.不同赋存状态页岩油定量表征技术与应用研究[J].石油实验地质,2016,38(6):842-849.JIANG Qigui,LI Maowen,QIAN Menhui,et al.Quantitative characterization of shale oil in different occurrence states and its application[J].Petroleum Geology&Experiment,2016,38(6):842-849.
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[12] RAHMAN H M,KENNEDY M,LHR S,et al.Clay-organic association as a control on hydrocarbon generation in shale[J]. Organic Geochemistry,2017,105:42-55.
[13] WU L M,ZHOU C H,KEELING J,et al. Towards an understanding of the role of clay minerals in crude oil formation,migration and accumulation[J]. Earth-Science Reviews,2012,115(4):373-386.
[14] ZEGOUAGH Y,DERENNE S,LARGEAU D,et al.A geochemical investigation of carboxylic acids released via sequential treatments of two surficial sediments from the Changjiang Delta and East China Sea[J]. Organic Geochemistry,2000,31(5):375-388.
[15]钱门辉,蒋启贵,黎茂稳,等.湖相页岩不同赋存状态的可溶有机质定量表征[J].石油实验地质,2017,39(2):278-286.QIAN Menhui,JIANG Qigui,LI Maowen,et al.Quantitative characterization of extractable organic matter in lacustrine shale with different occurrences[J]. Petroleum Geology&Experiment,2017,39(2):278-286.
[16]徐旭辉,郑伦举,马中良.泥页岩中有机质的赋存形态与油气形成[J].石油实验地质,2016,38(4):423-428.XU Xuhui,ZHENG Lunju,MA Zhongliang.Organic matter occurrence and hydrocarbon generation in shale[J].Petroleum Geology&Experiment,2016,38(4):423-428.
[17]张爽,隋微波.页岩储层有机质分布定量分析及重构模型[J].油气地质与采收率,2016,23(2):22-28.ZHANG Shuang,SUI Weibo.Reconstruction and quantitative analysis methods for organic matter distribution in shale reservoirs[J].Petroleum Geology and Recovery Efficiency,2016,23(2):22-28.
[18]刘天琳,姜振学,刘伟伟,等.江西修武盆地早寒武世热液活动对有机质富集的影响[J].油气地质与采收率,2018,25(3):68-76.LIU Tianlin,JIANG Zhenxue,LIU Weiwei,et al.Effect of hydrothermal activity on the enrichment of sedimentary organic matter at Early Cambrian in the Xiuwu Basin[J]. Petroleum Geology and Recovery Efficiency,2018,25(3):68-76.
[19]张钰莹,何治亮,高波,等.上扬子区下寒武统富有机质页岩沉积环境及其对有机质含量的影响[J].石油实验地质,2017,39(2):154-161.ZHANG Yuying,HE Zhiliang,GAO Bo,et al.Sedimentary environment of the Lower Cambrian organic-rich shale and its influence on organic content in the Upper Yangtze[J]. Petroleum Geology&Experiment,2017,39(2):154-161.
[20] LI Y L,CAI J G,WANG X J,et al.Smectite-illitization difference of source rocks developed in saline and fresh water environments and its influence on hydrocarbon generation:a study from the Shahejie Formation,Dongying Depression,China[J].Marine and Petroleum Geology,2017,80:349-357.
[21] ZHANG L Y,LIU Q,ZHU R F,et al.Source rocks in MesozoicCenozoic continental rift basins,East China:a case from Dongying Depression,Bohai Bay Basin[J]. Organic Geochemistry,2009,40(2):229-242.
[22]张林晔,孔祥星,张春荣,等.济阳坳陷下第三系优质烃源岩的发育及其意义[J].地球化学,2003,32(1):35-42.ZHANG Linye,KONG Xiangxing,ZHANG Chunrong,et al.Highquality oil-prone source rocks in Jiyang Depression[J]. Geochimica,2003,32(1):35-42.
[23]彼得斯K E,沃尔特斯C C,莫尔多万J M.生物标志化合物指南版.张水昌,李振西,译.北京:石油工业出版社,2011.PETERS K E,WALTERS C C,MOLDOWAN J M.The biomarker guide[M].2nd ed.ZHANG Shuichang,LI Zhenxi,trans.Beijing:Petroleum Industry Press,2011.
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