气候变化领域集成服务门户(CCPortal): Isotope Rollover of Gaseous Hydrocarbons Induced by Water Pressure in Laboratory Pyrolysis Experiments: Insights into the Influence of Pressure on Carbon Kinetic Isotope Effects During Methane Generation

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DOI	10.1007/s11053-022-10052-9
	Isotope Rollover of Gaseous Hydrocarbons Induced by Water Pressure in Laboratory Pyrolysis Experiments: Insights into the Influence of Pressure on Carbon Kinetic Isotope Effects During Methane Generation
	Wu, Yuandong; Li, Yuanju; Wang, Changfeng; Sun, Lina; Zhang, Zhongning; Ji, Liming; Zhang, Mingzhen; Su, Long
通讯作者	Li, YJ (通讯作者)，South China Univ Technol, Sch Mol Sci & Engn, Guangzhou 510641, Peoples R China. ; Li, YJ (通讯作者)，Shanwei Inst Technol, Shanwei 516600, Peoples R China.
发表日期	2020
ISSN	1520-7439
EISSN	1573-8981
英文摘要	Stable carbon isotope (delta C-13) rollover of natural gas has attracted recent attention due to its association with highly productive shale gas. However, the mechanistic causes of delta C-13 rollover are not fully understood. In this investigation, pyrolysis was carried out using calcareous shale and carbonaceous mudstone under high water pressure (WP) (i.e., 5 x 10(6)-1.2 x 10(8) Pa). It was found that WP induced the isotope rollover of gaseous hydrocarbons. For both sapropelic and humic organic matter, the delta C-13 rollover of CH4 (methane), C2H6 (ethane), and C3H8 (propane) occurred when the WP ranged from 3.25 x 10(7) to 1.2 x 10(8) Pa. This result can be explained by high WP conditions retarding oil cracking, and enhancing hydrocarbon expulsion and oil generation. The promotion of oil generation resulted in increasing trends of vitrinite reflectance, and inhibition of gaseous hydrocarbons generation resulted in decrease in delta C-13(1) values with increase in WP. Good functions were found between water pressure and the calculated carbon kinetic isotope effect (KIE) for (CH4)-C-12 and (CH4)-C-13 produced from sapropelic and humic organic matter. Further calculations showed that the increments of activation volume (Delta V-12CH2(double dagger) - Delta V-13CH4(double dagger)) were linearly corre- lated with the kinetic isotope effect of methane (Delta KIE) produced from sapropelic and humic organic matter, indicating that WP may affect the KIE of (CH4)-C-12 and (CH4)-C-13 by changing the Delta V-double dagger of (CH4)-C-12 and (CH4)-C-13. Overall, these findings suggest that WP affects the carbon isotope fractionation of gaseous hydrocarbons due to the different thermodynamic properties of (CH4)-C-12 and (CH4)-C-13.
关键词	HYDROUS PYROLYSIS THERMAL-CRACKING GAS GENERATION SHALE GAS FUEL-OIL FRACTIONATION EXPULSION KEROGEN ETHANE BASIN
英文关键词	Gaseous hydrocarbon; Isotope rollover; Kinetic isotope effect; Carbon isotope fractionation; Activation volume; (CH4)-C-12 and (CH4)-C-13
语种	英语
WOS研究方向	Geology
WOS类目	Geosciences, Multidisciplinary
WOS记录号	WOS:000782735300001
来源期刊	NATURAL RESOURCES RESEARCH
来源机构	中国科学院西北生态环境资源研究院
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/255026
作者单位	[Wu, Yuandong] Peking Univ, Shenzhen Inst, Shenzhen 518055, Peoples R China; [Li, Yuanju] South China Univ Technol, Sch Mol Sci & Engn, Guangzhou 510641, Peoples R China; [Li, Yuanju] Shanwei Inst Technol, Shanwei 516600, Peoples R China; [Wang, Changfeng] Huabei Petr Tiancheng Ind Grp Co Ltd, Renqiu 062550, Hebei, Peoples R China; [Sun, Lina] Yangtze Univ, Hubei Cooperat Innovat Ctr Unconvent Oil & Gas, Wuhan 430100, Hubei, Peoples R China; [Zhang, Zhongning; Ji, Liming; Zhang, Mingzhen; Su, Long] Chinese Acad Sci, Northwest Inst Ecoenvironm & Resources, Lanzhou 730000, Peoples R China; [Zhang, Zhongning; Ji, Liming; Zhang, Mingzhen; Su, Long] Key Lab Petr Resources, Lanzhou 730000, Gansu, Peoples R China; [Wu, Yuandong] Dongguan Univ Technol, Res Ctr Ecoenvironm Engn, Dongguan 523808, Peoples R China
推荐引用方式 GB/T 7714	Wu, Yuandong,Li, Yuanju,Wang, Changfeng,et al. Isotope Rollover of Gaseous Hydrocarbons Induced by Water Pressure in Laboratory Pyrolysis Experiments: Insights into the Influence of Pressure on Carbon Kinetic Isotope Effects During Methane Generation[J]. 中国科学院西北生态环境资源研究院,2020.
APA	Wu, Yuandong.,Li, Yuanju.,Wang, Changfeng.,Sun, Lina.,Zhang, Zhongning.,...&Su, Long.(2020).Isotope Rollover of Gaseous Hydrocarbons Induced by Water Pressure in Laboratory Pyrolysis Experiments: Insights into the Influence of Pressure on Carbon Kinetic Isotope Effects During Methane Generation.NATURAL RESOURCES RESEARCH.
MLA	Wu, Yuandong,et al."Isotope Rollover of Gaseous Hydrocarbons Induced by Water Pressure in Laboratory Pyrolysis Experiments: Insights into the Influence of Pressure on Carbon Kinetic Isotope Effects During Methane Generation".NATURAL RESOURCES RESEARCH (2020).