塔里木盆地麦盖提斜坡罗斯2井奥陶系油气藏的TSR作用:来自分子标志物的证据
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摘要
采用内标物色谱质谱方法,对罗斯2井原油中金刚烷系列、二苯并噻吩系列和硫代金刚烷系列进行了定量分析。罗斯2井原油中金刚烷系列化合物含量、4-甲基双金刚烷+3-甲基双金刚烷含量分别为10 818,331μg/g,表明原油经历了较强的裂解作用,裂解比例达到90%左右。金刚烷指标表明原油成熟度在1.6%以上。罗斯2井原油可以检测到完整的硫代单金刚烷、硫代双金刚烷和硫代三金刚烷系列,硫代金刚烷、硫代单金刚烷、硫代双金刚烷和硫代三金刚烷含量分别为192,160,26和6μg/g。高含量的硫代金刚烷表明罗斯2井原油的TSR强度大于绝大多数塔中地区下奥陶统鹰山组原油。TSR作用导致罗斯2井原油具有较高含量的二苯并噻吩,含量为8 201μg/g,使得原油二苯并噻吩/菲比值(DBT/P)增加,导致C_0-/C_1-DBTs和C_1-/C_2-DBTs比值增加。
The study made a quantitative analysis of diamondoid,dibenzothiophenes and thiadiamondoid series in the crude oil from Well Luosi-2 via the GC-MS method with internal standards.The concentrations of diamondoid and 4-+3-methyldiamantane( 4-+3-MD) are 10818 and 331 g/g in the study area,suggesting that the crude oil suffered serious cracking and the proportion of cracking oil is up to about 90%.The diamondoid indexes show that the maturity of crude oil from Well Luosi-2 is above 1. 6% R_c. Complete thiaadamantane,thiadiamantane,thiatriamantane series were detected from the Well Luosi-2 crude oil,with the contents of thiadiamondoid,thiaadamantane,thiadiamantane,thiatriamantane being 192,160,26 and 6 μg/g respectively.The high concentration of thiadiamondoid is a sign that the degree of thermochemical sulfate reduction( TSR) of oil from Well Luosi-2 is higher than that of most crude oil from the Lower Ordovician Yingshan Formation in Tazhong uplift.TSR results in the higher DBTs,about 8 201 μg/g,in the oil from Well Luosi-2,and in turn the higher ratios of DBT/P,C_0-/C_1-DBT and C_1-/C_2-DBT.
The study made a quantitative analysis of diamondoid,dibenzothiophenes and thiadiamondoid series in the crude oil from Well Luosi-2 via the GC-MS method with internal standards.The concentrations of diamondoid and 4-+3-methyldiamantane( 4-+3-MD) are 10818 and 331 g/g in the study area,suggesting that the crude oil suffered serious cracking and the proportion of cracking oil is up to about 90%.The diamondoid indexes show that the maturity of crude oil from Well Luosi-2 is above 1. 6% R_c. Complete thiaadamantane,thiadiamantane,thiatriamantane series were detected from the Well Luosi-2 crude oil,with the contents of thiadiamondoid,thiaadamantane,thiadiamantane,thiatriamantane being 192,160,26 and 6 μg/g respectively.The high concentration of thiadiamondoid is a sign that the degree of thermochemical sulfate reduction( TSR) of oil from Well Luosi-2 is higher than that of most crude oil from the Lower Ordovician Yingshan Formation in Tazhong uplift.TSR results in the higher DBTs,about 8 201 μg/g,in the oil from Well Luosi-2,and in turn the higher ratios of DBT/P,C_0-/C_1-DBT and C_1-/C_2-DBT.
引文
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[12]朱心健,陈践发,贺礼文,等.塔里木盆地麦盖提斜坡罗斯2井油气地球化学特征及油气源分析[J].天然气地球科学,2017,28(4):566-574.Zhu Xinjian,Chen Jianfa,He Liwen,et al.Geochemical characteristics and source correlation of hydrocarbons in the Well Luosi 2 of Maigaiti Slope,Tarim Basin,China[J].Natural Gas Geoscience,2017,28(4):566-574.
[13]Chen Junhong,Fu Jiamo,Shen Guoying,et al.,Diamondoid hydrocarbon ratios:Novel maturity indices for highly mature crude oils[J].Organic Geochemistry,1996,25(3/4):179-190.
[14]马安来.金刚烷类化合物在有机地球化学中的应用进展[J].天然气地球科学,2016,27(5):851-860.Ma Anlai.New advancement in application of diamondoids on organic geochemistry[J].Natural Gas Geoscience,2016,27(5):851-860.
[15]Dahl J E,Moldowan J M,Peter K E,et al.Diamondoid hydrocarbons as indicators of natural oil cracking[J].Nature,1999,399(5):54-56.
[16]王广利,李宁熙,高波,等.麻江奥陶系古油藏中硫酸盐热化学还原反应:来自分子标志物的证据[J].科学通报,2013,58(33):3450-3457.Wang Guangli,Li Ningxi,Gao Bo,et al.Thermochemical sulfate reduction in fossil Ordovician deposits of the Majiang area:Evidence from a molecular-marker investigation[J].Chinese Science Bulletin,2013,58(33):3450-3457.
[17]Cai Chunfang,Xiao Qilin,Fang Chenchen,et al.The effect of thermochemical sulfate reduction on formation and isomerization of thiadiamondoids and diamondoids in the Lower Paleozoic petroleum pools of the Tarim Basin,NW China[J].Organic Geochemistry,2016,101:49-62.
[18]马安来,金之钧,朱翠山,等.塔河油田原油中金刚烷化合物绝对定量分析[J].石油学报,2009,30(2):214-218.Ma Anlai,Jin Zhijun,Zhu Cuishan,et al.,Quantitative analysis on absolute concentration of diamondoids in oils from Tahe oilfield[J].Acta Petrolei Sinica,2009,30(2):214-218.
[19]马安来,金之钧,朱翠山.塔里木盆地塔河油田奥陶系原油成熟度及裂解程度研究[J].天然气地球科学,2017,28(2):313-323.Ma Anlai,Jin Zhijun,Zhu Cuishan.Maturity and oil-cracking of the Ordovician oils from Tahe Oilfield,Tarim Basin,NW China[J].Natural Gas Geoscience,2017,28(2):313-323.
[20]Hanin S,Adam P,Kowalewski I,et al.,Bridgehead alkylated 2-thiaadamantanes:a novel markers for sulfurization processes occurring under high thermal stress in deep petroleum reservoirs[J].Journal of Chemical Society,Chemical Communications,2002,1750-1751.
[21]Wei Zhibin.Molecular organic geochemistry of cage compounds and biomarkers in the geosphere:a novel approach to understand petroleum evolution and alteration[D].California:Stanford University,2006.
[22]Wei Zhibin,C.C.Walters,J.M.Moldowan,et al.,Thiadiamondoids as proxies for the extent of thermochemical sulfate reduction[J].Organic Geochemistry,2012,44:53-70.
[23]姜乃煌,朱光有,张水昌等.塔里木盆地塔中83井原油中检测出2-硫代金刚烷及其地质意义[J].科学通报,2007,52(24):2871-2875.Jiang Naihuang,Zhu Guangyou,Zhang Shuichang,et al.,Detection of2-thiaadamantanes in the oil from Well TZ-83 in Tarim Basin and its geological implication[J].Chinese Science Bulletin,2007,52(24):2871-2875.
[24]Zhu Guangyou,Wang Huitong,Weng Na.TSR-altered oil with high-abundance thiaadamantanes of a deep-buried Cambrian gas condensate reservoir in Tarim Basin[J].Marine and Petroleum Geology,2016,69:1-12.
[25]马安来,金之钧,朱翠山.塔里木盆地顺南1井原油硫代金刚烷系列的检出及意义[J].石油学报,2018,39(1):42-53.Ma Anlai,Jin Zhijun,Zhu Cuishan.Detection and research significance of thiadiamondoids from crude oil in Well Shunnan 1,Tarim Basin[J].Acta Petrolei Sinica,39(1):42:53.
[26]Wei Zhibin,Moldowan J M,Fago F,et a.,Origin of thiadiamondoids and diamondoidthiols in petroleum[J].Energy&Fuels,2007,21:3431-3436.
[27]Sinninghe Damste J S,Eglinton T L,de Leeuw J W,et al.,Organic Sulphur in macromolecular sedimentary organic matter.Part I.Structure and origin of Sulphur-containing moieties in kerogen,asphaltene and coal as revealed by flash pyrolysis[J].Geochimica et Cosmochimica Acta,1989,53:873-889.
[28]Hughes W B,Holba A G,Dzou L I.The ratios of dibenzothiophene to phenanthrene and pristine to phytane as indicators of depositional environment and lithology of petroleum source[J].Geochimica et Cosmochimica Acta,1995,59(17):3581-3598.
[29]Manzano B K,Fowler M G,Machel H G.The influence of thermochemical sulfate reduction on hydrocarbon composition in Nisku reservoirs,Brzaeau River area,alverta,Canada[J].Organic Geochemistry,1997,27:507-521.
[30]Zhang Shuichang,Su Jin,Huang Haiping,et al.,Genetic origin of sour gas condensates in the Paleozoic dolomite reservoirs of the Tazhong Uplift,Tarim Basin[J].Marine and Petroleum Geology,2015,68:107-119.
[31]Zhang Shuichang,Huang Haiping.Geochemistry of Palaeozoic marine petroleum from the Tarim Basin,NW China:Part 1.Oil family classification[J].Organic Geochemistry,2005,36:1204-1214.
[32]Zhang Shuichang,Huang Haiping,Su Jin,et al.,Geochemistry of Paleozoic marine petroleum from the Tarim Basin,NW China:Part 5.Effect of maturation,TSR and mixing on the occurrence and distribution of alkyldibenzothiophenes[J].Organic Geochemistry,2015,86:5-18.
[2]Worden R H,Smallwy P C,Oxtoby N H.Gas souring by thermochemical sulfate reduction at 140℃[J].AAPG Bulletin,1995,79(6):854-863.
[3]Machel H G,Krouse H R,Sassen R.Prodcuts and distinguishing criteria of bacterial and thermochemical sulfate reduction[J].Applied Geochemistry,1995,10(4):373-389.
[4]Cai C F,Worden R H,Wang Q F,et al.,Chemical and isotopic evidence for secondary alteration of natural gases in the Hetianhe Field,Bachu Uplift of the Tarim Basin[J].Organic Geochemistry,2002,33:1415-1427.
[5]Zhu G Y,Zhang S C,Liang Y B,et al.,Isotopic evidence of TSR origin for natural gas bearing high H2S content within Feixianguan Formation of the Northeastern Sichuan Basin,southwest China[J].Science in China Series D:Earth Science,2005,48(11):1037-1046.
[6]朱光有,费安国,赵杰,等.TSR成因H2S的硫同位素分馏特征与机制[J].岩石学报,2014,30(12):3772-3786.Zhu Guangyou,Fei Anguo,Zhao Jie,et al.,Sulfur isotopic fractionation and mechanism for thermochemical sulfate reduction genetic H2S[J].Acta Petrologica Sinica,2014,30(12):3772-3786.
[7]Walter C C,Wang F C,Qian Kuangnan,et al.,Petroleum alteration by thermochemical sulfate reduction:A comprehensive molecular study of aromatic hydrocarbons and polar compounds[J].Geochimica et Cosomochimica Acta,2015,153:37-71.
[8]Amrani A,Deev A,Sessions A L,et al.,The sulfur-isotopic compositions of benzothiophenes and dibenzothiophenes as a proxy for thermochemical sulfate reduction[J].Geochimica et Cosmochimica Acta,2012,84:152-164.
[9]Li Sumei,Amrani A,Pang Xiongqi,et al.,Origin and quantitative source assessment of deep oils in the Tazhong Uplift,Tarim Basin[J].Organic Geochemistry,2015,78:1-22.
[10]Gvirtzman Z,Said-Ahmad W,Ellis G S,et al.,Compound-specific sulfur isotope analysis of thiadiamondoids of oils from the Smackover Formation,USA[J].Geochimica et Cosmochimica Acta,2015,167:144-161.
[11]Cai Chunfang,Amrani A,Worden R H,et al.,Sulfur isotopic composition of individual organosulfur compounds and their genetic links in the Lower Paleozoic petroleum pools of the Tarim Basin,NW China[J].Geochimica et Cosmochimica Acta,2016,182:88-108.
[12]朱心健,陈践发,贺礼文,等.塔里木盆地麦盖提斜坡罗斯2井油气地球化学特征及油气源分析[J].天然气地球科学,2017,28(4):566-574.Zhu Xinjian,Chen Jianfa,He Liwen,et al.Geochemical characteristics and source correlation of hydrocarbons in the Well Luosi 2 of Maigaiti Slope,Tarim Basin,China[J].Natural Gas Geoscience,2017,28(4):566-574.
[13]Chen Junhong,Fu Jiamo,Shen Guoying,et al.,Diamondoid hydrocarbon ratios:Novel maturity indices for highly mature crude oils[J].Organic Geochemistry,1996,25(3/4):179-190.
[14]马安来.金刚烷类化合物在有机地球化学中的应用进展[J].天然气地球科学,2016,27(5):851-860.Ma Anlai.New advancement in application of diamondoids on organic geochemistry[J].Natural Gas Geoscience,2016,27(5):851-860.
[15]Dahl J E,Moldowan J M,Peter K E,et al.Diamondoid hydrocarbons as indicators of natural oil cracking[J].Nature,1999,399(5):54-56.
[16]王广利,李宁熙,高波,等.麻江奥陶系古油藏中硫酸盐热化学还原反应:来自分子标志物的证据[J].科学通报,2013,58(33):3450-3457.Wang Guangli,Li Ningxi,Gao Bo,et al.Thermochemical sulfate reduction in fossil Ordovician deposits of the Majiang area:Evidence from a molecular-marker investigation[J].Chinese Science Bulletin,2013,58(33):3450-3457.
[17]Cai Chunfang,Xiao Qilin,Fang Chenchen,et al.The effect of thermochemical sulfate reduction on formation and isomerization of thiadiamondoids and diamondoids in the Lower Paleozoic petroleum pools of the Tarim Basin,NW China[J].Organic Geochemistry,2016,101:49-62.
[18]马安来,金之钧,朱翠山,等.塔河油田原油中金刚烷化合物绝对定量分析[J].石油学报,2009,30(2):214-218.Ma Anlai,Jin Zhijun,Zhu Cuishan,et al.,Quantitative analysis on absolute concentration of diamondoids in oils from Tahe oilfield[J].Acta Petrolei Sinica,2009,30(2):214-218.
[19]马安来,金之钧,朱翠山.塔里木盆地塔河油田奥陶系原油成熟度及裂解程度研究[J].天然气地球科学,2017,28(2):313-323.Ma Anlai,Jin Zhijun,Zhu Cuishan.Maturity and oil-cracking of the Ordovician oils from Tahe Oilfield,Tarim Basin,NW China[J].Natural Gas Geoscience,2017,28(2):313-323.
[20]Hanin S,Adam P,Kowalewski I,et al.,Bridgehead alkylated 2-thiaadamantanes:a novel markers for sulfurization processes occurring under high thermal stress in deep petroleum reservoirs[J].Journal of Chemical Society,Chemical Communications,2002,1750-1751.
[21]Wei Zhibin.Molecular organic geochemistry of cage compounds and biomarkers in the geosphere:a novel approach to understand petroleum evolution and alteration[D].California:Stanford University,2006.
[22]Wei Zhibin,C.C.Walters,J.M.Moldowan,et al.,Thiadiamondoids as proxies for the extent of thermochemical sulfate reduction[J].Organic Geochemistry,2012,44:53-70.
[23]姜乃煌,朱光有,张水昌等.塔里木盆地塔中83井原油中检测出2-硫代金刚烷及其地质意义[J].科学通报,2007,52(24):2871-2875.Jiang Naihuang,Zhu Guangyou,Zhang Shuichang,et al.,Detection of2-thiaadamantanes in the oil from Well TZ-83 in Tarim Basin and its geological implication[J].Chinese Science Bulletin,2007,52(24):2871-2875.
[24]Zhu Guangyou,Wang Huitong,Weng Na.TSR-altered oil with high-abundance thiaadamantanes of a deep-buried Cambrian gas condensate reservoir in Tarim Basin[J].Marine and Petroleum Geology,2016,69:1-12.
[25]马安来,金之钧,朱翠山.塔里木盆地顺南1井原油硫代金刚烷系列的检出及意义[J].石油学报,2018,39(1):42-53.Ma Anlai,Jin Zhijun,Zhu Cuishan.Detection and research significance of thiadiamondoids from crude oil in Well Shunnan 1,Tarim Basin[J].Acta Petrolei Sinica,39(1):42:53.
[26]Wei Zhibin,Moldowan J M,Fago F,et a.,Origin of thiadiamondoids and diamondoidthiols in petroleum[J].Energy&Fuels,2007,21:3431-3436.
[27]Sinninghe Damste J S,Eglinton T L,de Leeuw J W,et al.,Organic Sulphur in macromolecular sedimentary organic matter.Part I.Structure and origin of Sulphur-containing moieties in kerogen,asphaltene and coal as revealed by flash pyrolysis[J].Geochimica et Cosmochimica Acta,1989,53:873-889.
[28]Hughes W B,Holba A G,Dzou L I.The ratios of dibenzothiophene to phenanthrene and pristine to phytane as indicators of depositional environment and lithology of petroleum source[J].Geochimica et Cosmochimica Acta,1995,59(17):3581-3598.
[29]Manzano B K,Fowler M G,Machel H G.The influence of thermochemical sulfate reduction on hydrocarbon composition in Nisku reservoirs,Brzaeau River area,alverta,Canada[J].Organic Geochemistry,1997,27:507-521.
[30]Zhang Shuichang,Su Jin,Huang Haiping,et al.,Genetic origin of sour gas condensates in the Paleozoic dolomite reservoirs of the Tazhong Uplift,Tarim Basin[J].Marine and Petroleum Geology,2015,68:107-119.
[31]Zhang Shuichang,Huang Haiping.Geochemistry of Palaeozoic marine petroleum from the Tarim Basin,NW China:Part 1.Oil family classification[J].Organic Geochemistry,2005,36:1204-1214.
[32]Zhang Shuichang,Huang Haiping,Su Jin,et al.,Geochemistry of Paleozoic marine petroleum from the Tarim Basin,NW China:Part 5.Effect of maturation,TSR and mixing on the occurrence and distribution of alkyldibenzothiophenes[J].Organic Geochemistry,2015,86:5-18.