Stable isotope reversal and evolution of gas during the hydrous pyrolysis of continental kerogen in source rocks under supercritical conditions
Wu, Yuandong1; Zhang, Zhongning2; Sun, Lina3; Li, Yuanju4; Zhang, Mingzheng2; Ji, Liming2
刊名INTERNATIONAL JOURNAL OF COAL GEOLOGY
2019-03-01
卷号205页码:105-114
关键词Stable isotope reversal Mixing Adsorption/desorption Shale gas Hydrous pyrolysis Semi-closed condition
ISSN号0166-5162
DOI10.1016/j.coal.2019.03.004
英文摘要Semi-closed hydrous pyrolysis experiments were conducted to investigate the isotopic evolution of shale gas produced from continental organic-rich shales with increasing thermal maturity and prospecting potential. The delta C-13 values of methane, ethane, propane and n-butane became heavier with increasing thermal maturity and showed good relationships with vitrinite reflectance (VR). Gases expelled from type-I, type-II, and type-III kerogens followed the normal carbon sequence (delta C-13(c1) < delta C-13(c2) < delta C-13(c3) < delta C-13(nc)4) and the hydrogen isotopic sequence (delta H-2(c1) < delta H-2(c2) < delta H-2(c3) < delta H-2(nc4) < delta H-2(IC)4) among the alkanes at VRs lower than 2.14% R-o, 2.42% R-o, and 1.87% R-o respectively. The isotopically reversed gases (delta C-13(c1) < delta C-13(c2) < delta C-13(nc4) < delta C-13(c3)) were observed in type-I kerogen with a VRs above 2.14% R-o and in type-II kerogen with a VR above 2.42% R-o. In type-III kerogen, isotopically reversed gases (delta C-13(c1) < delta C-13(nc4) < delta C-13(c3) < delta C-13(c2)) were observed with a VR above 2.94% Ro. These results suggest four stages in the stable carbon isotope reversal of ethane, propane, and n-butane with increasing maturity. The isotopically reversed gases (delta C-13(c1) < delta C-13(c2) < delta C-13(nc4) < delta C-13(c3)) may represent lower maturity and higher productivity shale gas than the isotopically reversed gases (delta C-13(c1) < delta C-13(nc4) < delta C-13(c3) < delta C-13(c2)), indicating that continental type-I kerogen has the highest potential productivity for shale gas, and continental type-III kerogen has the lowest. Stable hydrogen isotope composition did not respond to the stable carbon isotope reversal in isotopically reversed gases. We suggest that indigenous generation and mixing may be the dominant mechanisms responsible for the stable carbon isotope reversal, and adsorption/desorption during hydrocarbon expulsion may promote the stable isotope reversal under semi-closed conditions. Overall, these results suggest that this study is an important contribution to continental shale gas exploration.
资助项目China Postdoctoral Science Foundation[2018M643618] ; National Science and Technology Major Projects of Ministry of Science and Technology of China[2016ZX05007001-004] ; Key Laboratory Project of Gansu Province[1309RTSA041]
WOS关键词TRIASSIC YANCHANG FORMATION ; CLOSED-SYSTEM PYROLYSIS ; HYDROCARBON GENERATION ; NATURAL GASES ; SHALE-GAS ; ORDOS BASIN ; GEOCHEMICAL CHARACTERISTICS ; MISSISSIPPIAN BARNETT ; THERMAL MATURITY ; METHANE
WOS研究方向Energy & Fuels ; Geology
语种英语
出版者ELSEVIER SCIENCE BV
WOS记录号WOS:000464298600008
资助机构China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; National Science and Technology Major Projects of Ministry of Science and Technology of China ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province ; Key Laboratory Project of Gansu Province
内容类型期刊论文
源URL[http://ir.iggcas.ac.cn/handle/132A11/91280]  
专题地质与地球物理研究所_兰州油气中心
通讯作者Zhang, Zhongning
作者单位1.Dongguan Univ Technol, Res Ctr Ecoenvironm Engn, Dongguan 523808, Peoples R China
2.Chinese Acad Sci, Inst Geol & Geophys, Key Lab Petr Resources, Gansu Prov Key Lab Petr Resources Res, Lanzhou 730000, Gansu, Peoples R China
3.Yangtze Univ, Hubei Cooperat Innovat Ctr Unconvent Oil & Gas, Wuhan 430100, Hubei, Peoples R China
4.Peking Univ, Sch Environm & Eneriy, Shenzhen 518055, Peoples R China
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Wu, Yuandong,Zhang, Zhongning,Sun, Lina,et al. Stable isotope reversal and evolution of gas during the hydrous pyrolysis of continental kerogen in source rocks under supercritical conditions[J]. INTERNATIONAL JOURNAL OF COAL GEOLOGY,2019,205:105-114.
APA Wu, Yuandong,Zhang, Zhongning,Sun, Lina,Li, Yuanju,Zhang, Mingzheng,&Ji, Liming.(2019).Stable isotope reversal and evolution of gas during the hydrous pyrolysis of continental kerogen in source rocks under supercritical conditions.INTERNATIONAL JOURNAL OF COAL GEOLOGY,205,105-114.
MLA Wu, Yuandong,et al."Stable isotope reversal and evolution of gas during the hydrous pyrolysis of continental kerogen in source rocks under supercritical conditions".INTERNATIONAL JOURNAL OF COAL GEOLOGY 205(2019):105-114.
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