四川盆地二叠系不同类型烃源岩生烃热模拟实验
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摘要
通过对四川盆地二叠系不同类型烃源岩(泥质灰岩、沥青灰岩、泥岩和煤)在加水封闭体系下的热模拟实验,结果表明不同类型干酪根之间产气率明显不同。Ⅰ型干酪根的泥质灰岩总产气率最高(4226m3/tTOC),其次为沥青灰岩(2 445.5 m3/tTOC),煤岩总产气率最低(459.3 m3/tTOC),Ⅲ型干酪根的泥岩总产气率高于煤岩。泥质灰岩烃类气体产率仍然最高(765 m3/tTOC),其次为泥岩(606.1 m3/tTOC),沥青灰岩最低。泥岩烃类气体产率高于沥青灰岩,可能与沥青灰岩中除去烃类遭受热裂解外,碳酸盐分解生成大量非烃气体(CO2)有关,从而造成总产气率高,而烃类气体产率却偏低的现象。这样,沥青灰岩生成的烃类主要来源于分散有机质热裂解,而不是灰岩本身。不同类型气源生烃对比结果表明,Ⅰ型干酪根的泥质灰岩或Ⅲ型干酪根的泥岩有利于低温生烃,而煤岩和分散有机质生烃历程长,有利于后期天然气生成与聚集保存。
Different types of the Permian source rocks(argillaceous limestone,asphaltic limestone,shale and coal) in Sichuan basin with 10mLwater were subjected to isothermal pyrolysis in a seal stainless steel reactor at temperatures ranging from 300℃ to 550℃ with 50℃ intervals for a duration of 24 h.Gas yield vary significantly for the different types of source rocks.Total gas yield from argillaceous limestone as type Ⅰ kerogen(maximum value=4 226 m3/tTOC) is much higher than those from other source rocks,then from asphaltic limestone(maximum value=2 445.5 m3/tTOC).Coal has the lowest gas yield(maximum value=459.3 m3/tTOC).The total gas yield from shale as type Ⅲ kerogen is more than that from coal.The maximum yield of total hydrocarbon gas is from argillaceous limestone(765 m3/tTOC),then from shale(606.1 m3/tTOC).Similar yields of hydrocarbon gas from coal,crude oil and asphaltic limestone occur.The case that hydrocarbon gas yield from shale is higher than that from asphaltic limestone would be related to the generation of non-hydrocarbon gas(i.e.CO2) from thermal decomposition of carbonates besides hydrocarbons cracking in asphaltic limestone.Thus,the total gas yield from asphaltic limestone is relatively high,but the hydrocarbon gas yield comparatively low,suggesting that the hydrocarbon gas from asphaltic limestone would greatly stem from the thermal cracking of the dispersed soluble organic matter but not from the asphaltic limestone itself.By comparison among the gas yields from different source rocks,it can be concluded that argillaceous limestone as kerogen Ⅰ or shale as kerogen Ⅲ is in favor of hydrocarbon generation at low temperature,whereas coal and dispersed soluble organic matter have a long-term period of hydrocarbon generation,and thus generation of hydrocarbon gas from coal and dispersed soluble organic matter is good for hydrocarbons accumulation later.
Different types of the Permian source rocks(argillaceous limestone,asphaltic limestone,shale and coal) in Sichuan basin with 10mLwater were subjected to isothermal pyrolysis in a seal stainless steel reactor at temperatures ranging from 300℃ to 550℃ with 50℃ intervals for a duration of 24 h.Gas yield vary significantly for the different types of source rocks.Total gas yield from argillaceous limestone as type Ⅰ kerogen(maximum value=4 226 m3/tTOC) is much higher than those from other source rocks,then from asphaltic limestone(maximum value=2 445.5 m3/tTOC).Coal has the lowest gas yield(maximum value=459.3 m3/tTOC).The total gas yield from shale as type Ⅲ kerogen is more than that from coal.The maximum yield of total hydrocarbon gas is from argillaceous limestone(765 m3/tTOC),then from shale(606.1 m3/tTOC).Similar yields of hydrocarbon gas from coal,crude oil and asphaltic limestone occur.The case that hydrocarbon gas yield from shale is higher than that from asphaltic limestone would be related to the generation of non-hydrocarbon gas(i.e.CO2) from thermal decomposition of carbonates besides hydrocarbons cracking in asphaltic limestone.Thus,the total gas yield from asphaltic limestone is relatively high,but the hydrocarbon gas yield comparatively low,suggesting that the hydrocarbon gas from asphaltic limestone would greatly stem from the thermal cracking of the dispersed soluble organic matter but not from the asphaltic limestone itself.By comparison among the gas yields from different source rocks,it can be concluded that argillaceous limestone as kerogen Ⅰ or shale as kerogen Ⅲ is in favor of hydrocarbon generation at low temperature,whereas coal and dispersed soluble organic matter have a long-term period of hydrocarbon generation,and thus generation of hydrocarbon gas from coal and dispersed soluble organic matter is good for hydrocarbons accumulation later.
引文
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[19]Liu Wenhui,Zhang Jianyong,Fan Ming,et al.Gas generationcharacter of dissipated soluble organic matter[J].Petroleum Geol-ogy&Experiment,2007,29(1):1-6.[刘文汇,张建勇,范明,等.叠合盆地天然气的重要来源———分散可溶有机质[J].石油实验地质,2007,29(1):1-6.]
[2]Tissot B T,Durand B,Espitalie J,et al.Influence of nature anddiagenesis of organic matter in formation of petroleum[J].AAPGBulletin,1974,58(3):499-506.
[3]Hansford R C.Mechanisms of Some Hydrocarbon Reactions[M]//Farkas A.Physical Chemistry of the Hydrocarbon.NewYork:Academic Press,1953:187-318.
[4]Liu Quanyou,Liu Wenhui,Song Yan,et al.Characteristics of liq-uid hydrocarbon for Tarim coal and its macerals in thermal pyroly-sis experiments[J].Natural Gas Geoscience,2004,15(3):97-101.[刘全有,刘文汇,宋岩,等.塔里木盆地煤岩显微组分热模拟实验中液态烃特征研究[J].天然气地球科学,2004,15(3):97-101.]
[5]Schenk HJ,Horsfield B.Kinetics of petroleum generation by pro-grammed-temperature closed-versus open-system pyrolysis[J].Geochimica et Cosmochimica Acta,1993,57(3):623-630.
[6]Mango F D,Hightower J W,James A T.Role of transition-metalcatalysis in the formation of natural gas[J].Nature,1994,368(6471):536-538.
[7]Mango F D.The stability of hydrocarbons under the time-tempera-ture condition of petroleum genesis[J].Nature,1991,352(6331):146-148.
[8]Liu Quanyou,Liu Wenhui,Qin Shengfei,et al.Geochemical studyof thermal simulation of coal and coal adding different mediums-rate of gaseous and organic liquid products and the evolution char-acteristics[J].Acta Sedimentological Sinica,2001,19(3):465-468.[刘全有,刘文汇,秦胜飞,等.煤岩及煤岩加不同介质的热模拟地球化学实验———气态和液态产物的产率以及演化特征[J].沉积学报,2001,19(3):465-468.]
[9]Cramer B,Faber E,Gerling P,et al.Reaction kinetics of stablecarbon isotopes in natural gas-insights from dry,open system py-rolysis experiment[J].Energy&Fuels,2001,15(3):517-532.
[10]Tang Y,Behar F.Rate constants of n-alkanes generation fromtypeII kerogen in open and closed pyrolysis systems[J].Energy&Fu-els,1995,9(3):507-512.
[11]Berner U,Faber E,Scheeder G,et al.Primary cracking of algaland landplant kerogen:kinetic models of isotope variations inmethane,ethane and propane[J].Chemical Geology,1995,126(3-4):233-245.
[12]Chen Anding,Zhang Wenzheng,Xu Yongchang.Isotope character-istics and its application of products from hydrocarbon generatingthermal simulation experiments on sedimentary rock[J].Sciencein China:Series B,1993,23(2):209-217.[陈安定,张文正,徐永昌.沉积岩成烃热模拟实验产物的同位素特征及应用[J].中国科学:B辑,1993,23(2):209-217.]
[13]Cheng Keming,Wang Zhaoyun.An evaluation method of hydro-carbon generating potential of highly mature and over-mature ma-rine carbonate[J].Science in China:Series D,1997,40(1):81-90.[程克明,王兆云.高成熟和过成熟海相碳酸盐岩生烃条件评价方法研究[J].中国科学:D辑,1996,26(6):537-543.]
[14]Liu Quanyou,Liu Wenhui,Dai Jinxing.Characterization of pyroly-sates from maceral components of Tarim coals in closed system ex-periments and implications to natural gas generation[J].OrganicGeochemistry,2007,38(6):921-934.
[15]Saxby J D,Riley K W.Petroleum generation by laboratoty scalepyrolysis over six years simulating conditions in a subsiding basin[J].Nature,1984,308(5955):177-179.
[16]Ma Yongsheng.Geochemical characteristics and origin of naturalgases from Puguang gas field on eastern Sichuan basin[J].Natu-ral Gas Geoscience,2008,19(1):1-7.[马永生.普光气田天然气地球化学特征及气源探讨[J].天然气地球科学,2008,19(1):1-7.
[17]Qin Jianzhong.Hydrocarbon Sources in Chinese Sedimentary Ba-sins[M].Beijing:Science Press,2005:1-618.[秦建中.中国烃源岩[M].北京:科学出版社,2005:1-618.]
[18]Liu Quanyou.Permian Hydrocarbon Source and Key ConditionsConstrained the Marine Upper Assemblage Gas Reservoirs in Si-chuan Basin[R].Beijing:Exploration&Production Research In-stitute,SINOPEC,Post Doctor Thesis,2009:1-213.[刘全有.四川盆地二叠系烃源岩评价与海相上组合天然气成藏主控因素研究[R].北京:中国石油化工股份有限公司石油勘探开发研究院,博士后出站报告,2009:1-213.]
[19]Liu Wenhui,Zhang Jianyong,Fan Ming,et al.Gas generationcharacter of dissipated soluble organic matter[J].Petroleum Geol-ogy&Experiment,2007,29(1):1-6.[刘文汇,张建勇,范明,等.叠合盆地天然气的重要来源———分散可溶有机质[J].石油实验地质,2007,29(1):1-6.]
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