一种解释高-过成熟烷烃气碳同位素系列倒转的新观点：芳香烃脱甲基作用

彭威龙; 刘全有; 胡国艺; 吕玥; 孟庆强; 郭丰涛; 关海洋

doi:10.3799/dqkx.2019.133

Volume 45 Issue 4

Apr. 2020

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Article Navigation > Earth Science > 2020 > 45(4): 1308-1314

Peng Weilong, Liu Quanyou, Hu Guoyi, Lü Yue, Meng Qingqiang, Guo Fengtao, Guan Haiyang, 2020. A New Interpretation of Carbon Isotope Series Reverse of Highly-Over Mature Alkane Gases: Demethylation of Aromatic Hydrocarbons. Earth Science, 45(4): 1308-1314. doi: 10.3799/dqkx.2019.133

Citation:

Peng Weilong, Liu Quanyou, Hu Guoyi, Lü Yue, Meng Qingqiang, Guo Fengtao, Guan Haiyang, 2020. A New Interpretation of Carbon Isotope Series Reverse of Highly-Over Mature Alkane Gases: Demethylation of Aromatic Hydrocarbons. Earth Science, 45(4): 1308-1314. doi: 10.3799/dqkx.2019.133

Citation:

Peng Weilong, Liu Quanyou, Hu Guoyi, Lü Yue, Meng Qingqiang, Guo Fengtao, Guan Haiyang, 2020. A New Interpretation of Carbon Isotope Series Reverse of Highly-Over Mature Alkane Gases: Demethylation of Aromatic Hydrocarbons. Earth Science, 45(4): 1308-1314. doi: 10.3799/dqkx.2019.133

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A New Interpretation of Carbon Isotope Series Reverse of Highly-Over Mature Alkane Gases: Demethylation of Aromatic Hydrocarbons

doi: 10.3799/dqkx.2019.133

1.
State Key Laboratory of Shale Oil and Gas Enrichment Mechanisms and Effective Development, SINOPEC, Beijing 100083, China
2.
Petroleum Exploration and Production Research Institute, SINOPEC, Beijing 100083, China
3.
Research Institute of Petroleum Exploration & Development, PetroChina, Beijing 100083, China
4.
Exploration and Development Research Institute of Liaohe Oilfield Company, CNPC, Panjin 124010, China

Received Date: 2019-06-04
Publish Date: 2020-04-15

Abstract

Abstract

The genetic mechanism of natural gas is complex. In view of the fact that carbon isotope series reverse of alkane gas exists generally in the highly-over mature stage, and the organic matter in the highly-over mature stage is often rich in aromatic ring structure, the carbon isotope series reverse of alkane gas in the highly-over mature stage is discussed by means of pyrolysis experiments of aromatic hydrocarbons (toluene). The pyrolysis of toluene shows that the yield of alkane gas increases with the increase of simulated temperature, and the yield of H₂ in the product increases with the increase of simulated temperature. The distribution ranges of δ¹³C₁, δ¹³C₂ and δ¹³C₃ in toluene pyrolysis products are -31.8‰ to -27.7‰, -31.0‰ to -20.4‰ and -31.0‰ to -20.4‰, respectively. In the toluene thermal simulation experiment at 450℃, partial reversal of carbon isotope series of alkanes occurred (δ¹³C₁>δ¹³C₂ < δ¹³C₃). It is found that carbon isotope series reversal occurs in both coal type gas and oil type gas at highly-over mature stage. Combining with the simulation results, it is considered that aromatic hydrocarbon demethylation may be an important reason for carbon isotope series reversal in highly-over mature stage of alkane gas.
- thermal simulation experiment,
- natural gas,
- carbon isotope,
- aromatic hydrocarbon pyrolysis,
- toluene,
- hydrocarbons

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References(53)

References

Cai, Y.W., Zhang, S.C., He, K., et al., 2017.The Effect of Magnetite on the Products and Isotopic Fractions of Gaseous Hydrocarbons. Natural Gas Geoscience, 28(2):331-340 (in Chinese with English abstract). http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201702017

Dai, J.X., 1992. Identification of Alkane Gas. Science China Earth Sciences, 2:185-193 (in Chinese). http://d.old.wanfangdata.com.cn/Periodical/sp201803018

Dai, J. X., Ni, Y. Y., Huang, S. P., et al., 2016a. Secondary Origin of Negative Carbon Isotopic Series in Natural Gas. Journal of Natural Gas Geoscience, 1(1):1-7. https://doi.org/10.1016/j.jnggs.2016.02.002

Dai, J. X., Xia, X. Y., Qin, S. F., et al., 2004. Origins of Partially Reversed Alkane δ¹³C Values for Biogenic Gases in China. Organic Geochemistry, 35(4):405-411. https://doi.org/10.1016/j.orggeochem.2004.01.006

Dai, J. X., Zou, C. N., Dong, D. Z., et al., 2016b. Geochemical Characteristics of Marine and Terrestrial Shale Gas in China. Marine and Petroleum Geology, 76:444-463. https://doi.org/10.1016/j.marpetgeo.2016.04.027

Dai, J. X., Zou, C. N., Liao, S. M., et al., 2014. Geochemistry of the Extremely High Thermal Maturity Longmaxi Shale Gas, Southern Sichuan Basin. Organic Geochemistry, 74:3-12. https://doi.org/10.1016/j.orggeochem.2014.01.018

Dai, J.X., Pei, X.G., Qi, H.F., 1992. Natural Gas Geology in China (Vol.1). Petroleum Industry Press, Beijing, 116-129 (in Chinese).

Feng, Z.Q., Dong, D.Z., Tian, J. Q., et al., 2018. Geochemical Characteristics of Longmaxi Formation Shale Gas in the Weiyuan Area, Sichuan Basin, China. Journal of Petroleum Science and Engineering, 167:538-548. https://doi.org/10.1016/j.petrol.2018.04.030

Galimov, E. M., 2006. Isotope Organic Geochemistry. Organic Geochemistry, 37(10):1200-1262. https://doi.org/10.1016/j.orggeochem.2006.04.009

Gao, B., 2015.Geochemical Characteristics of Shale Gas from Lower Silurian Longmaxi Formation in the Sichuan Basin and Its Geological Significance. Natural Gas Geoscience, 26(6):1173-1182 (in Chinese with English abstract). http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201506019

Hill, R. J., Jarvie, D. M., Zumberge, J., et al., 2007. Oil and Gas Geochemistry and Petroleum Systems of the Fort Worth Basin. AAPG Bulletin, 91(4):445-473. https://doi.org/10.1306/11030606014

Hill, R. J., Tang, Y. C., Kaplan, I. R., 2003. Insights into Oil Cracking Based on Laboratory Experiments. Organic Geochemistry, 34(12):1651-1672. https://doi.org/10.1016/s0146-6380(03)00173-6

Hu, G.Y., Li, J., Li, Z.S., et al., 2010.Composition and Carbon Isotopic Distribution Characteristics of Light Hydrocarbon in Coal-Derived Gas and Natural Gas Exploration. Acta Petrolei Sinica, 31(1):42-48(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=syxb201001007

Hunt, J., 1979. Petroleum Geochemistry and Geology. Freeman and Company, New York.

Li, J., Li, J., Li, Z. S., et al., 2014. The Hydrogen Isotopic Characteristics of the Upper Paleozoic Natural Gas in Ordos Basin. Organic Geochemistry, 74:66-75. https://doi.org/10.1016/j.orggeochem.2014.01.020

Liu, Q. Y., Jin, Z. J., Li, H. L., et al., 2018. Geochemistry Characteristics and Genetic Types of Natural Gas in Central Part of the Tarim Basin, NW China. Marine and Petroleum Geology, 89:91-105. https://doi.org/10.1016/j.marpetgeo.2017.05.002

Liu, Q. Y., Worden, R. H., Jin, Z. J., et al., 2013. TSR versus Non-TSR Processes and Their Impact on Gas Geochemistry and Carbon Stable Isotopes in Carboniferous, Permian and Lower Triassic Marine Carbonate Gas Reservoirs in the Eastern Sichuan Basin, China. Geochimica et Cosmochimica Acta, 100:96-115. https://doi.org/10.1016/j.gca.2012.09.039

Liu, Q. Y., Worden, R. H., Jin, Z. J., et al., 2014. Thermochemical Sulphate Reduction (TSR) versus Maturation and Their Effects on Hydrogen Stable Isotopes of very Dry Alkane Gases. Geochimica et Cosmochimica Acta, 137:208-220. https://doi.org/10.1016/j.gca.2014.03.013

Liu, Q. Y., Wu, X. Q., Wang, X. F., et al., 2019. Carbon and Hydrogen Isotopes of Methane, Ethane, and Propane:A Review of Genetic Identification of Natural Gas. Earth-Science Reviews, 190:247-272. https://doi.org/10.1016/j.earscirev.2018.11.017

Mi, J. K., Zhang, S. C., He, K., 2014. Experimental Investigations about the Effect of Pressure on Gas Generation from Coal. Organic Geochemistry, 74:116-122. https://doi.org/10.1016/j.orggeochem.2014.05.012

Mi, J. K., Zhang, S. C., Su, J., et al., 2018. The Upper Thermal Maturity Limit of Primary Gas Generated from Marine Organic Matters. Marine and Petroleum Geology, 89:120-129. https://doi.org/10.1016/j.marpetgeo.2017.06.045

Peng, W. L., Hu, G. Y., Liu, Q. Y., et al., 2018. Research Status on Thermal Simulation Experiment and Several Issues of Concern. Journal of Natural Gas Geoscience, 3(5):283-293. https://doi.org/10.1016/j.jnggs.2018.11.006

Qin, S.F., 2012.Carbon Isotopic Composition of Water-Soluble Gases and Its Geological Significance in the Sichuan Basin. Petroleum Exploration and Development, 39(3):313-319(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=syktykf201203007

Schoell, M., 1980. The Hydrogen and Carbon Isotopic Composition of Methane from Natural Gases of Various Origins. Geochimica et Cosmochimica Acta, 44(5):649-661. https://doi.org/10.1016/0016-7037(80)90155-6

Schoell, M., 1983. Genetic Characterization of Natural Gas. AAPG Bulletin, 67:2225-2238. http://d.old.wanfangdata.com.cn/Periodical/ycxb201308008

Song, Z.X., Gu, Y., Lu, Q.H., et al., 2016.Genetic Types of Natural Gas and Its Exploration Direction in Lishu Fault Sag, Songliao Basin. Acta Petrolei Sinica, 37(5):622-630(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=syxb201605006

Sun, M.L., Liu, G.D., 2013.Genesis Type and Source Analysis in Lower Cretaceous of Changling Depression in Songliao Basin.Geoscience, 27(5):1186-1192(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=xddz201305022

Tang, Y., Perry, J. K., Jenden, P. D., et al., 2000. Mathematical Modeling of Stable Carbon Isotope Ratios in Natural Gases. Geochimica et Cosmochimica Acta, 64(15):2673-2687. https://doi.org/10.1016/s0016-7037(00)00377-x

Tang, G.M., Luo, Q., Pang, X.Q., et al., 2014.Natural Gas Genetic Type and Accumulation Characteristics in Erboliang Ⅲ Structure in North Margin of Qaidam Basin. Xinjiang Petroleum Geology, 35(1):17-22(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=xjsydz201401005

Tissot, B.P., Welte, D.H., 1984. Petroleum Formation and Occurrence(Second Edition). Springer-Verlag, Berlin, Heidelberg, New York, Tokyo.

Wang, D.L., Zhang, Y., Lu, S.F., et al., 2012.The Simulation Experiment on Gas-Generating Potential of Over Mature Source Rocks. Acta Sedimentologica Sinica, 30(6):1172-1179(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cjxb201206022

Wang, J., Chen, J.F., Wang, T.G., et al., 2006.Gas Source Rocks and Gas Genetic Type in Shuangcheng-Taipingchuan Area of Songliao Basin. Acta Petrolei Sinica, 27(3):16-21(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=syxb200603004

Wei, X.F., Guo, T.L., Liu, R.B., et al., 2016.Geochemical Features of Shale Gas and Their Genesis in Jiaoshiba Block of Fuling Shale Gasfield, Chongqing. Natural Gas Geoscience, 27(3):539-548(in Chinese with English abstract). http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201603017

Yu, C., Gong, D.Y., Huang, S.P., et al., 2014.Geochemical Characteristics of Carbon and Hydrogen Isotopes for the Xujiahe Formation Natural Gas in Sichuan Basin. Natural Gas Geoscience, 25(1):87-97(in Chinese with English abstract). http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201401010

Zhai, L.N., Ni, Y.Y., Wu, C.D., et al., 2017.Geochemical Characteristics of the Natural Gas from the Xujiahe Formation in the Central Sichuan Basin, China. Natural Gas Geoscience, 28(4):539-549(in Chinese with English abstract). http://www.en.cnki.com.cn/Article_en/CJFDTOTAL-TDKX201704008.htm

Zhang, J., Zhao, H.J., Zhang, M., et al., 2012.Geochemical Characteristics and Origin of Natural Gas in Lishu Fault Depression, Songliao Basin. Petroleum Geology & Experiment, 34(4):417-421(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=sysydz201204013

Zhao, L.B., Huang, Z.L., Ma, Y.J., et al., 2006.A Study on Geochemical Character and Origin of Deep Natural Gas in Dehui Fault Depression of the Southern Songliao Basin. Natural Gas Geoscience, 17(2):177-182(in Chinese with English abstract). http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=trqdqkx200602009

蔡郁文, 张水昌, 何坤, 等, 2017.磁铁矿对有机质生烃及同位素分馏的影响.天然气地球科学, 28(2):331-340. http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201702017

戴金星, 1992.各类烷烃气的鉴别.中国科学:地球科学, 2:185-193. http://www.cqvip.com/qk/88064X/199202/985597.html

戴金星, 裴锡古, 戚厚发, 1992.中国天然气地质学(卷一).北京: 石油工业出版社, 116-129.

高波, 2015.四川盆地龙马溪组页岩气地球化学特征及其地质意义.天然气地球科学, 26(6):1173-1182. http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201506019

胡国艺, 李谨, 李志生, 等, 2010.煤成气轻烃组分和碳同位素分布特征与天然气勘探.石油学报, 31(1):42-48. http://d.old.wanfangdata.com.cn/Periodical/syxb201001007

秦胜飞, 2012.四川盆地水溶气碳同位素组成特征及地质意义.石油勘探与开发, 39(3):313-319. http://d.old.wanfangdata.com.cn/Periodical/syktykf201203007

宋振响, 顾忆, 路清华, 等, 2016.松辽盆地梨树断陷天然气成因类型及勘探方向.石油学报, 37(5):622-630. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=syxb201605006

孙明亮, 柳广弟, 2013.松辽盆地长岭断陷下白垩统天然气成因及气源分析.现代地质, 27(5):1186-1192. doi: 10.3969/j.issn.1000-8527.2013.05.022

汤国民, 罗群, 庞雄奇, 等, 2014.柴北缘鄂博梁Ⅲ号构造天然气成因类型及其成藏特征.新疆石油地质, 35(1):17-22. http://d.old.wanfangdata.com.cn/Periodical/xjsydz201401005

王东良, 张英, 卢双舫, 等, 2012.烃源岩过成熟阶段生气潜力的实验室模拟.沉积学报, 30(6):1172-1179. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cjxb201206022

王杰, 陈践发, 王铁冠, 等, 2006.松辽盆地双城-太平川地区天然气成因类型及气源.石油学报, 27(3):16-21. doi: 10.3321/j.issn:0253-2697.2006.03.004

魏祥峰, 郭彤楼, 刘若冰, 等, 2016.涪陵页岩气田焦石坝地区页岩气地球化学特征及成因.天然气地球科学, 27(3):539-548. http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201603017

于聪, 龚德瑜, 黄士鹏, 等, 2014.四川盆地须家河组天然气碳、氢同位素特征及其指示意义.天然气地球科学, 25(1):87-97. http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201401010

翟俪娜, 倪云燕, 吴朝东, 等, 2017.川中地区须家河组天然气地球化学特征.天然气地球科学, 28(4):539-549. http://d.old.wanfangdata.com.cn/Periodical/trqdqkx201704006

张俊, 赵红静, 张敏, 等, 2012.松辽盆地梨树断陷天然气地球化学特征及成因探讨.石油实验地质, 34(4):417-421. doi: 10.3969/j.issn.1001-6112.2012.04.013

赵力彬, 黄志龙, 马玉杰, 等, 2006.松辽盆地南部德惠断陷深层天然气地球化学特征及成因.天然气地球科学, 17(2):177-182. doi: 10.3969/j.issn.1672-1926.2006.02.009

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A New Interpretation of Carbon Isotope Series Reverse of Highly-Over Mature Alkane Gases: Demethylation of Aromatic Hydrocarbons

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