四川盆地中部三叠系须家河组煤成气丁烷和戊烷的异正构比与成熟度关系
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摘要
以四川盆地中部三叠系须家河组不同地区和不同层位原生气藏为对象,采用常规天然气地球化学研究方法,探讨煤成气组分中iC_4/nC_4和iC_5/nC_5值与成熟度之间关系。通过对8个气田73个天然气样品研究发现,煤成气中iC_4/nC_4和iC_5/nC_5值具有一致的变化规律,即呈良好的正相关关系,复相关系数大于0.8。iC_4/nC_4和iC_5/nC_5值随天然气干燥系数(C_1/C_(1+))变高、甲烷碳同位素组成变重而呈有规律地增大,它们之间具有较高的相关性。该研究揭示了煤系生成重烃异构体变化特性,提出了煤成气成熟度的新指标:iC_4/nC_4及iC_5/nC_5值与计算的Ro值之间的回归方程,为煤成气成熟度的判定、天然气运移、后期改造以及成藏等研究都提供了重要参考依据。图7表1参29
The original gas reservoirs in different areas and different layers of the Triassic Xujiahe Formation in the central Sichuan Basin are studied to reveal the relationships of iC_4/nC_4 and iC_5/nC_5 ratios in coal-derived gas components with maturity using conventional natural gas geochemical research methods. The testing results of 73 gas samples from 8 gas fields show that the iC_4/nC_4 and iC_5/nC_5 ratios in coal-derived gas have a good positive correlation, and the correlation coefficient is above 0.9. Both the iC_4/nC_4 and iC_5/nC_5 ratios become higher with the increase of natural gas dryness coefficient(C_1/C_(1+)) and the methane carbon isotope becoming less negative. These parameters are highly correlated. This study not only reveals characteristics of heavy hydrocarbon isomers generated by coal formation, but also puts forward new identification indicators reflecting the maturity of coal-derived gas, the regression between iC_4/nC_4, iC_5/nC_5 and Ro, which can provide an important reference for maturity, migration and accumulation of coal-derived gas, and late stage reformation of coal-derived gas reservoirs.
The original gas reservoirs in different areas and different layers of the Triassic Xujiahe Formation in the central Sichuan Basin are studied to reveal the relationships of iC_4/nC_4 and iC_5/nC_5 ratios in coal-derived gas components with maturity using conventional natural gas geochemical research methods. The testing results of 73 gas samples from 8 gas fields show that the iC_4/nC_4 and iC_5/nC_5 ratios in coal-derived gas have a good positive correlation, and the correlation coefficient is above 0.9. Both the iC_4/nC_4 and iC_5/nC_5 ratios become higher with the increase of natural gas dryness coefficient(C_1/C_(1+)) and the methane carbon isotope becoming less negative. These parameters are highly correlated. This study not only reveals characteristics of heavy hydrocarbon isomers generated by coal formation, but also puts forward new identification indicators reflecting the maturity of coal-derived gas, the regression between iC_4/nC_4, iC_5/nC_5 and Ro, which can provide an important reference for maturity, migration and accumulation of coal-derived gas, and late stage reformation of coal-derived gas reservoirs.
引文
[1]戴金星.中国煤成气理论研究30年来勘探重大进展[J].石油勘探与开发,2009,36(3):264-279.DAI Jinxing.Major developments of coal-formed gas exploration in the last 30 years in China[J].Petroleum Exploration and Development,2009,36(3):264-279.
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[3]赵文智,王红军,钱凯.中国煤成气理论发展及其在天然气工业发展中的地位[J].石油勘探与开发,2009,36(3):280-288.ZHAO Wenzhi,WANG Hongjun,QIAN Kai.Progress of coal-formed gas geological theory and its status in natural gas industry in China[J].Petroleum Exploration and Development,2009,36(3):280-288.
[4]张福东,李君,魏国齐,等.低生烃强度区致密砂岩气形成机制:以鄂尔多斯盆地天环坳陷北段上古生界为例[J].石油勘探与开发,2018,45(1):73-81.ZHANG Fudong,LI Jun,WEI Guoqi,et al.Formation mechanism of tight sandstone gas in areas of low hydrocarbon generation intensity:A case study of the Upper Paleozoic in North Tianhuan Depression in Ordos Basin,NW China[J].Petroleum Exploration and Development,2018,45(1):73-81.
[5]STAHL W J,GARE B D.Source-rock identification by isotope analyses of natural gases from field in the Val Verde and Delaware Basins,West Texas[J].Chemical Geology,1975,16(4):257-267.
[6]戴金星,戚厚发.我国煤成烃气的δ13C-Ro关系[J].科学通报,1989,34(9):690-692.DAI Jinxing,QI Houfa.δ13C-Ro relationship of coal derived gas in China[J].Chinese Science Bulletin,1989,34(9):690-692.
[7]刘文汇,徐永昌.煤型气碳同位素演化二阶段分馏模式及机理[J].地球化学,1999,28(4):359-366.LIU Wenhui,XU Yongchang.A two stage model of carbon isotopic fractionation in coal gas[J].Geochimica,1999,28(4):359-366.
[8]戴金星,倪云燕,张文正,等.中国煤成气湿度和成熟度关系[J].石油勘探与开发,2016,43(5):675-678.DAI Jinxing,NI Yunyan,ZHANG Wenzheng,et al.Relationships between wetness and maturity of coal-derived gas in China[J].Petroleum Exploration and Development,2016,43(5):675-678.
[9]秦胜飞,戴金星,王兰生.川西前陆盆地次生气藏天然气来源追踪[J].地球化学,2007,36(4):368-374.QIN Shengfei,DAI Jinxing,WANG Lansheng.Different origins of natural gas in secondary gas pool in Western Sichuan foreland basin[J].Geochimica,2007,36(4):368-374.
[10]叶素娟,朱宏权,李嵘,等.天然气运移有机-无机地球化学示踪指标:以四川盆地川西坳陷侏罗系气藏为例[J].石油勘探与开发,2017,44(4):549-560.YE Sujuan,ZHU Hongquan,LI Rong,et al.Tracing natural gas migration by integrating organic and inorganic geochemical data:Acase study of the Jurassic gas fields in western Sichuan Basin,SWChina[J].Petroleum Exploration and Development,2017,44(4):549-560.
[11]郝石生,黄志龙,杨家琦.天然气运聚动平衡及其应用[M].北京:石油工业出版社,1994:12-13.HAO Shisheng,HUANG Zhilong,YANG Jiaqi.The migrationaccumulation equilibrium theory and application of natural gas[M].Beijing:Petroleum Industry Press,1994:12-13.
[12]王鹏,沈忠民,何崇康,等.天然气中丁烷地球化学特征及应用[J].天然气地球科学,2017,28(4):529-538.WANG Peng,SHEN Zhongmin,HE Chongkang,et al.The geochemical characteristics of butane and its application[J].Natural Gas Geoscience,2017,28(4):529-538.
[13]李广之,吴向华.异构比φiC4/φnC4和φiC5/φnC5的石油地质意义[J].物探与化探,2002,26(2):135-139.LI Guangzhi,WU Xianghua.The petroleum geological significance of somerization ratesφiC4/φnC4 andφiC5/φnC5[J].Geophysical&Geochemical Exploration,2002,26(2):135-139.
[14]QIN S F,ZHANG Y H,ZHAO C Y,et al.Geochemical evidence for in situ accumulation of tight gas in the Xujiahe Formation coal measures in the central Sichuan Basin,China[J].International Journal of Coal Geology,2018,196:173-184.
[15]徐樟有,宋丽,吴欣松,等.川中地区上三叠统须家河组典型气藏解剖与天然气成藏主控因素分析[J].岩性油气藏,2009,21(2):7-11.XU Zhangyou,SONG Li,WU Xinsong,et al.Typical gas reservoir and main controlling factors of reservoir-forming of Upper Triassic Xujiahe Formation in central Sichuan Basin[J].Lithologic Reservoirs,2009,21(2):7-11.
[16]王威,徐国盛,雍自权,等.川中地区香四段气水分布特征及成因机理[J].成都理工大学学报(自然科学版),2005,32(4):378-382.WANG Wei,XU Guosheng,YONG Ziquan,et al.Distribution rule and formation mechanism of gas and water in Layer 4 of Xiangxi Group of the central area in Sichuan,China[J].Journal of Chengdu University of Technology(Science&Technology Edition),2005,32(4):378-382.
[17]杨威,谢增业,金惠,等.四川盆地上三叠统须家河组储层评价及天然气成藏机理[J].天然气工业,2010,30(12):10-15.YANG Wei,XIE Zengye,JIN Hui,et al.Reservoir evaluation and pooling mechanism of the Xujiahe formation in the Sichuan Basin[J].Natural Gas Industry,2010,30(12):10-15.
[18]张响响,邹才能,朱如凯,等.川中地区上三叠统须家河组储层成岩相[J].石油学报,2011,32(2):257-264.ZHANG Xiangxiang,ZOU Caineng,ZHU Rukai,et al.Reservoir diagenetic facies of the Upper Triassic Xujiahe Formation in the central Sichuan Basin[J].Acta Petrolei Sinica,2011,32(2):257-264.
[19]DAI Jinxing.Giant coal-derived gas fields and their gas sources in China[M].Beijing:Science Press,2016.
[20]戴金星,钟宁宁,刘德汉,等.中国煤成大中型气田地质基础和主控因素[M].北京:石油工业出版社,2000.DAI Jinxing,ZHONG Ningning,LIU Dehan,et al.Geological basis and controlling factors of large and medium gas fields in China[M].Beijing:Petroleum Industry Press,2000.
[21]DAI J X,NI Y Y,ZOU C N.Stable carbon and hydrogen isotopes of natural gases sourced from the Xujiahe Formation in the Sichuan Basin,China[J].Natural Gas Geoscience,2012,43:103-111.
[22]李登华,李伟,汪泽成,等.川中广安气田天然气成因类型及气源分析[J].中国地质,2007,34(4):829-836.LI Denghua,LI Wei,WANG Zecheng,et al.Genetic type and source of gas in the Guang’an gas field,central Sichuan[J].Geology in China,2007,34(4):829-836.
[23]陶士振,邹才能,陶小晚,等.川中须家河组流体包裹体与天然气成藏机理[J].矿物岩石地球化学通报,2009,28(1):2-11.TAO Shizhen,ZOU Caineng,TAO Xiaowan,et al.Study on fluid and gas accumulation mechanism of Xujiahe Formation of Upper Triassic in the Sichuan Basin[J].Bulletin of Mineralogy,Petrology and Geochemistry,2009,28(1):2-11.
[24]QIN S F,LI F,LI W,et al.Formation mechanism of tight coal-derived-gas reservoirs with medium-low abundance in Xujiahe Formation,central Sichuan Basin,China[J].Marine and Petroleum Geology,2018,89:144-154.
[25]戴金星,倪云燕,胡国艺,等.中国致密砂岩大气田的稳定碳氢同位素组成特征[J].中国科学:地球科学,2014,44(4):563-578.DAI Jinxing,NI Yunyan,HU Guoyi,et al.Stable carbon and hydrogen isotopes of gases from the large tight gas fields in China[J].SCIENCE CHINA Earth Sciences,2014,57(1):88-103.
[26]WHITICAR M J.Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane[J].Chemical Geology,1999,161(1/2/3):291-314.
[27]林壬子.轻烃技术在油气勘探中的应用[M].武汉:中国地质大学出版社,1992.LIN Renzi.Application of light hydrocarbon technology in oil and gas exploration[M].Wuhan:China Geological University Press,1992.
[28]高岗,刚文哲,郝石生,等.腐殖煤气态产物演化特征的模拟实验研究[J].沉积学报,1998,16(2):30-33,41.GAO Gang,GANG Wenzhe,HAO Shisheng,et al.The evolution characteristics of gaseous products of humic coal and its geological significance[J].Acta Sedimentologica Sinica,1998,16(2):30-33,41.
[29]ZUMBERGE J,FERWORN K,BROWN S.Isotopic reversal(‘rollover’)in shale gases produced from the Mississippian Barnett and Fayetteville formations[J].Marine and Petroleum Geology,2012,31(1):43-52.
[2]戴金星,倪云燕,黄士鹏,等.煤成气研究对中国天然气工业发展的重要意义[J].天然气地球科学,2014,25(1):1-22.DAI Jinxing,NI Yunyan,HUANG Shipeng,et al.Significant function of coal-derived gas study for natural gas industry in China[J].Natural Gas Geoscience,2014,25(1):1-22.
[3]赵文智,王红军,钱凯.中国煤成气理论发展及其在天然气工业发展中的地位[J].石油勘探与开发,2009,36(3):280-288.ZHAO Wenzhi,WANG Hongjun,QIAN Kai.Progress of coal-formed gas geological theory and its status in natural gas industry in China[J].Petroleum Exploration and Development,2009,36(3):280-288.
[4]张福东,李君,魏国齐,等.低生烃强度区致密砂岩气形成机制:以鄂尔多斯盆地天环坳陷北段上古生界为例[J].石油勘探与开发,2018,45(1):73-81.ZHANG Fudong,LI Jun,WEI Guoqi,et al.Formation mechanism of tight sandstone gas in areas of low hydrocarbon generation intensity:A case study of the Upper Paleozoic in North Tianhuan Depression in Ordos Basin,NW China[J].Petroleum Exploration and Development,2018,45(1):73-81.
[5]STAHL W J,GARE B D.Source-rock identification by isotope analyses of natural gases from field in the Val Verde and Delaware Basins,West Texas[J].Chemical Geology,1975,16(4):257-267.
[6]戴金星,戚厚发.我国煤成烃气的δ13C-Ro关系[J].科学通报,1989,34(9):690-692.DAI Jinxing,QI Houfa.δ13C-Ro relationship of coal derived gas in China[J].Chinese Science Bulletin,1989,34(9):690-692.
[7]刘文汇,徐永昌.煤型气碳同位素演化二阶段分馏模式及机理[J].地球化学,1999,28(4):359-366.LIU Wenhui,XU Yongchang.A two stage model of carbon isotopic fractionation in coal gas[J].Geochimica,1999,28(4):359-366.
[8]戴金星,倪云燕,张文正,等.中国煤成气湿度和成熟度关系[J].石油勘探与开发,2016,43(5):675-678.DAI Jinxing,NI Yunyan,ZHANG Wenzheng,et al.Relationships between wetness and maturity of coal-derived gas in China[J].Petroleum Exploration and Development,2016,43(5):675-678.
[9]秦胜飞,戴金星,王兰生.川西前陆盆地次生气藏天然气来源追踪[J].地球化学,2007,36(4):368-374.QIN Shengfei,DAI Jinxing,WANG Lansheng.Different origins of natural gas in secondary gas pool in Western Sichuan foreland basin[J].Geochimica,2007,36(4):368-374.
[10]叶素娟,朱宏权,李嵘,等.天然气运移有机-无机地球化学示踪指标:以四川盆地川西坳陷侏罗系气藏为例[J].石油勘探与开发,2017,44(4):549-560.YE Sujuan,ZHU Hongquan,LI Rong,et al.Tracing natural gas migration by integrating organic and inorganic geochemical data:Acase study of the Jurassic gas fields in western Sichuan Basin,SWChina[J].Petroleum Exploration and Development,2017,44(4):549-560.
[11]郝石生,黄志龙,杨家琦.天然气运聚动平衡及其应用[M].北京:石油工业出版社,1994:12-13.HAO Shisheng,HUANG Zhilong,YANG Jiaqi.The migrationaccumulation equilibrium theory and application of natural gas[M].Beijing:Petroleum Industry Press,1994:12-13.
[12]王鹏,沈忠民,何崇康,等.天然气中丁烷地球化学特征及应用[J].天然气地球科学,2017,28(4):529-538.WANG Peng,SHEN Zhongmin,HE Chongkang,et al.The geochemical characteristics of butane and its application[J].Natural Gas Geoscience,2017,28(4):529-538.
[13]李广之,吴向华.异构比φiC4/φnC4和φiC5/φnC5的石油地质意义[J].物探与化探,2002,26(2):135-139.LI Guangzhi,WU Xianghua.The petroleum geological significance of somerization ratesφiC4/φnC4 andφiC5/φnC5[J].Geophysical&Geochemical Exploration,2002,26(2):135-139.
[14]QIN S F,ZHANG Y H,ZHAO C Y,et al.Geochemical evidence for in situ accumulation of tight gas in the Xujiahe Formation coal measures in the central Sichuan Basin,China[J].International Journal of Coal Geology,2018,196:173-184.
[15]徐樟有,宋丽,吴欣松,等.川中地区上三叠统须家河组典型气藏解剖与天然气成藏主控因素分析[J].岩性油气藏,2009,21(2):7-11.XU Zhangyou,SONG Li,WU Xinsong,et al.Typical gas reservoir and main controlling factors of reservoir-forming of Upper Triassic Xujiahe Formation in central Sichuan Basin[J].Lithologic Reservoirs,2009,21(2):7-11.
[16]王威,徐国盛,雍自权,等.川中地区香四段气水分布特征及成因机理[J].成都理工大学学报(自然科学版),2005,32(4):378-382.WANG Wei,XU Guosheng,YONG Ziquan,et al.Distribution rule and formation mechanism of gas and water in Layer 4 of Xiangxi Group of the central area in Sichuan,China[J].Journal of Chengdu University of Technology(Science&Technology Edition),2005,32(4):378-382.
[17]杨威,谢增业,金惠,等.四川盆地上三叠统须家河组储层评价及天然气成藏机理[J].天然气工业,2010,30(12):10-15.YANG Wei,XIE Zengye,JIN Hui,et al.Reservoir evaluation and pooling mechanism of the Xujiahe formation in the Sichuan Basin[J].Natural Gas Industry,2010,30(12):10-15.
[18]张响响,邹才能,朱如凯,等.川中地区上三叠统须家河组储层成岩相[J].石油学报,2011,32(2):257-264.ZHANG Xiangxiang,ZOU Caineng,ZHU Rukai,et al.Reservoir diagenetic facies of the Upper Triassic Xujiahe Formation in the central Sichuan Basin[J].Acta Petrolei Sinica,2011,32(2):257-264.
[19]DAI Jinxing.Giant coal-derived gas fields and their gas sources in China[M].Beijing:Science Press,2016.
[20]戴金星,钟宁宁,刘德汉,等.中国煤成大中型气田地质基础和主控因素[M].北京:石油工业出版社,2000.DAI Jinxing,ZHONG Ningning,LIU Dehan,et al.Geological basis and controlling factors of large and medium gas fields in China[M].Beijing:Petroleum Industry Press,2000.
[21]DAI J X,NI Y Y,ZOU C N.Stable carbon and hydrogen isotopes of natural gases sourced from the Xujiahe Formation in the Sichuan Basin,China[J].Natural Gas Geoscience,2012,43:103-111.
[22]李登华,李伟,汪泽成,等.川中广安气田天然气成因类型及气源分析[J].中国地质,2007,34(4):829-836.LI Denghua,LI Wei,WANG Zecheng,et al.Genetic type and source of gas in the Guang’an gas field,central Sichuan[J].Geology in China,2007,34(4):829-836.
[23]陶士振,邹才能,陶小晚,等.川中须家河组流体包裹体与天然气成藏机理[J].矿物岩石地球化学通报,2009,28(1):2-11.TAO Shizhen,ZOU Caineng,TAO Xiaowan,et al.Study on fluid and gas accumulation mechanism of Xujiahe Formation of Upper Triassic in the Sichuan Basin[J].Bulletin of Mineralogy,Petrology and Geochemistry,2009,28(1):2-11.
[24]QIN S F,LI F,LI W,et al.Formation mechanism of tight coal-derived-gas reservoirs with medium-low abundance in Xujiahe Formation,central Sichuan Basin,China[J].Marine and Petroleum Geology,2018,89:144-154.
[25]戴金星,倪云燕,胡国艺,等.中国致密砂岩大气田的稳定碳氢同位素组成特征[J].中国科学:地球科学,2014,44(4):563-578.DAI Jinxing,NI Yunyan,HU Guoyi,et al.Stable carbon and hydrogen isotopes of gases from the large tight gas fields in China[J].SCIENCE CHINA Earth Sciences,2014,57(1):88-103.
[26]WHITICAR M J.Carbon and hydrogen isotope systematics of bacterial formation and oxidation of methane[J].Chemical Geology,1999,161(1/2/3):291-314.
[27]林壬子.轻烃技术在油气勘探中的应用[M].武汉:中国地质大学出版社,1992.LIN Renzi.Application of light hydrocarbon technology in oil and gas exploration[M].Wuhan:China Geological University Press,1992.
[28]高岗,刚文哲,郝石生,等.腐殖煤气态产物演化特征的模拟实验研究[J].沉积学报,1998,16(2):30-33,41.GAO Gang,GANG Wenzhe,HAO Shisheng,et al.The evolution characteristics of gaseous products of humic coal and its geological significance[J].Acta Sedimentologica Sinica,1998,16(2):30-33,41.
[29]ZUMBERGE J,FERWORN K,BROWN S.Isotopic reversal(‘rollover’)in shale gases produced from the Mississippian Barnett and Fayetteville formations[J].Marine and Petroleum Geology,2012,31(1):43-52.