Evolution of carbon isotopic compositions for gas generated in semi-closed pyrolysis system: Reflections on the formation of isotopic abnormal gases
文献类型：期刊论文
| 作者 | Song, Dongjun1,3; Wu, Chenjun2; Tuo, Jincai1; Wang, Xiaoqi5; Zhang, Mingfeng1; He, Wei1,3; Ma, Zunqing4; Su, Long1; Jin, Xu5 |
| 刊名 | JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
 |
| 出版日期 | 2021-06-01 |
| 卷号 | 201页码:13 |
| ISSN号 | 0920-4105 |
| 关键词 | Shale gas Carbon isotope rollover Carbon isotope reversal Semi-closed pyrolysis Multiperiod preservation-loss processes |
| DOI | 10.1016/j.petrol.2021.108516 |
| 英文摘要 | Carbon isotope anomalies are signals for highly productive shale gas, but are poorly duplicated in completely closed or open pyrolysis systems. In this study, five low-maturity shale samples and one high-maturity shale sample were subjected to semi-closed pyrolysis experiments to investigate whether isotopically anomalous gases could be generated in laboratory simulations of the full maturity range. The results reveal that the first rollover of methane, ethane, and propane delta C-13 values occurs at the late oil-window stage, and the second rollover of delta C-13 (C2H6) and delta C-13(C3H8) values occurs at the overmature stage. Partial carbon isotopically reversed gases are produced, with isotope compositions evolving from delta C-13(C2H6) > delta C-13(C3H8) > delta C-13(CH4) through delta C-13(CH4) > delta C-13(C3H8) > delta C-13(C2H6) to delta C-13(C3H8) > delta C-13(CH4) > delta C-13(C2H6 as thermal maturity increases, whereas complete carbon isotopically reversed gases are not reproduced. These findings are slightly different from the carbon isotope and chemical characteristics of shale gas under natural conditions, which is universally characterized by full carbon isotope reversal. Compared to closed or open systems, the carbon isotopically anomalous gases are superimposed results of gaseous compounds from each episodic expulsion during semi-closed pyrolysis, illustrating that multiple periods of preservation and loss of gases are more important for carbon isotope reversal than thermal maturity. Carbon isotope fractionation via gas diffusion can be amplified by some large-scale processes of preservation and loss; for example, the uplift of a shale would lead to preferential diffusion of methane rich in C-12, resulting in full isotopic reversal in the residual gas in shales. These processes generally occur under natural conditions, but such factors have yet to be considered in conventional open or closed pyrolysis simulations. This study provides a reasonable reference for the issue of why (full) isotopically reversed gases can barely be produced in conventional pyrolysis experiments. |
| 资助项目 | National Natural Science Foundation of China[41672127] ; National Natural Science Foundation of China[41902143] ; National Natural Science Foundation of China[41602151] ; Natural Science Found of Gansu Province[17JR5RA293] ; National Key Research and Development Program of China[2019YFA0708701] |
| WOS研究方向 | Energy & Fuels ; Engineering |
| 语种 | 英语 |
| 出版者 | ELSEVIER |
| WOS记录号 | WOS:000628869500078 |
| 资助机构 | National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Found of Gansu Province ; Natural Science Found of Gansu Province ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Found of Gansu Province ; Natural Science Found of Gansu Province ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Found of Gansu Province ; Natural Science Found of Gansu Province ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Found of Gansu Province ; Natural Science Found of Gansu Province ; National Key Research and Development Program of China ; National Key Research and Development Program of China |
| 源URL | [http://ir.iggcas.ac.cn/handle/132A11/101068]  |
| 专题 | 地质与地球物理研究所_兰州油气中心 |
| 通讯作者 | Tuo, Jincai; Wang, Xiaoqi |
| 作者单位 | 1.Chinese Acad Sci, Northwest Inst Ecoenvironm & Resources, Key Lab Petr Resources, Lanzhou 730000, Gansu, Peoples R China 2.Yangtze Univ, Coll Resources & Environm, Wuhan 430100, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Nanjing Univ, Sch Earth Sci & Engn, Nanjing 210000, Peoples R China 5.Res Inst Petr Explorat & Dev, Beijing 10083, Peoples R China |
| 推荐引用方式 GB/T 7714 | Song, Dongjun,Wu, Chenjun,Tuo, Jincai,et al. Evolution of carbon isotopic compositions for gas generated in semi-closed pyrolysis system: Reflections on the formation of isotopic abnormal gases[J]. JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING,2021,201:13. |
| APA | Song, Dongjun.,Wu, Chenjun.,Tuo, Jincai.,Wang, Xiaoqi.,Zhang, Mingfeng.,...&Jin, Xu.(2021).Evolution of carbon isotopic compositions for gas generated in semi-closed pyrolysis system: Reflections on the formation of isotopic abnormal gases.JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING,201,13. |
| MLA | Song, Dongjun,et al."Evolution of carbon isotopic compositions for gas generated in semi-closed pyrolysis system: Reflections on the formation of isotopic abnormal gases".JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING 201(2021):13. |
入库方式： OAI收割
来源：地质与地球物理研究所
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