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名   称 Relationship between Hydrocarbon Gas Generation and Kerogen Structural Evolution Revealed by Closed System Pyrolysis and Quantitative Py-GC Analysis of a Type II Kerogen
科技资源标识 CSTR:11738.14.NCDC.XDA14.PP4452.2024
DOI 10.1021/acs.energyfuels.0c02468
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摘   要 Kerogen can release both liquid and gaseous hydrocarbons during thermal maturation. In this study, the maturation
and hydrocarbon generation of a low-maturity type II kerogen were simulated via temperature-programmed gold tube closed system
(GTCS) pyrolysis at two different heating rates. In addition to the yields of C1−C5 gaseous hydrocarbons, H/C atomic ratios and
δ13C values were also obtained on the kerogen residues from GTCS pyrolyses. The remaining C1−C5 gaseous hydrocarbon and C6
+
liquid hydrocarbon generation potentials in both the original kerogen and the kerogen residues of various thermal maturities were
determined by quantitative flash pyrolysis-gas chromatography (Py-GC) and were used to estimate the loss of aliphatic carbons in
artificially matured kerogens compared with that in the original kerogen. The yields of C1−C5 gaseous hydrocarbons from GTCS
pyrolysis were compared with the lost amount of C1−C5 gaseous hydrocarbon potentials within the kerogen structure at the same
maturities. The results indicate that the H/C atomic ratios of kerogen residues decreased and the δ13C values of kerogen residues
became progressively heavier (i.e., being enriched in 13C) with increasing maturity in the oil generation window (OGW) but with
δ13C becoming slightly lighter above the calculated Ro (Calcd Ro, namely, Easy Ro or equivalent vitrinite reflectance) of 2.5%. It is
worth noting that, in the OGW, the yields of C1−C5 gaseous hydrocarbons from GTCS pyrolyses were significantly lower than the
amounts of lost C1−C5 potentials indicated by Py-GC. We speculate that hydrocarbon gases generated in OGW may either be
partially adsorbed within kerogen and dissolved in oil or participate in the thermal degradation of kerogen during GTCS pyrolyses,
resulting in lower yields of C1−C5 gaseous hydrocarbons than the decrease in kerogen C1−C5 potentials. The Py-GC results of
kerogen residues also show that the rates of loss for C1, C2, and C3 hydrocarbons are about 92%, 98%, and 99%, respectively, at 1.3%
Calcd Ro. This indicates that most of the C2
+ alkyl side chains can be cleaved from the kerogen structure within OGW. In
comparison, at a Calcd Ro of 1.3%, the formation rate of methane (C1) from GTCS pyrolysis of kerogen at a heating rate of 2 °C/h
only amounted to about 32%. The results from this study appear to suggest that, in GTCS pyrolysis, most C1 generated from type II
kerogen at the overmature stage cannot be attributed to primary kerogen cracking but to gradual secondary cracking of hydrocarbons
with high molecular weights.
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作者 Yijun Zheng
数据量 4.9 MiB
论文类型: journal
论文网址: https://dx.doi.org/10.1021/acs.energyfuels.0c02468
期刊名称: Energy & Fuels
出版时间: 2021-09-01
引用和标注
数据引用
Yijun Zheng. Relationship between Hydrocarbon Gas Generation and Kerogen Structural Evolution Revealed by Closed System Pyrolysis and Quantitative Py-GC Analysis of a Type II Kerogen. 国家冰川冻土沙漠科学数据中心(http://www.ncdc.ac.cn), 2024. https://cstr.cn/CSTR:11738.14.NCDC.XDA14.PP4452.2024.
Yijun Zheng. Relationship between Hydrocarbon Gas Generation and Kerogen Structural Evolution Revealed by Closed System Pyrolysis and Quantitative Py-GC Analysis of a Type II Kerogen. 国家冰川冻土沙漠科学数据中心(http://www.ncdc.ac.cn), 2024. https://www.doi.org/10.1021/acs.energyfuels.0c02468.
许可协议
知识共享许可协议   本作品采用 知识共享署名 4.0 国际许可协议进行许可。

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