Thermal Transformation of Sulfur Species and Hydrogen Sulfide Formation in High-Pyrite-Containing Lacustrine Type-II Shale during Semiopen Pyrolysis
The shale of the seventh member of the Triassic Yanchang Formation in the Ordos Basin (abbreviated as Chang 7 shale) is the most prospective shale for in situ conversion process. In our previous study, a series of artificial maturation experiments were conducted to simulate the hydrocarbon generatio...
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| Veröffentlicht in: | Energy & fuels 2021-05, Vol.35 (9), p.7778-7786 |
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| creator | Ma, Weijiao Hou, Lianhua Luo, Xia Liu, Jinzhong Han, Wenxue |
| description | The shale of the seventh member of the Triassic Yanchang Formation in the Ordos Basin (abbreviated as Chang 7 shale) is the most prospective shale for in situ conversion process. In our previous study, a series of artificial maturation experiments were conducted to simulate the hydrocarbon generation–retention–expulsion process. However, during the experiments, a large amount of hydrogen sulfide (H2S) was generated along with hydrocarbon products. Therefore, in this study, a combination of X-ray photoelectron spectroscopy, X-ray diffraction, and elemental analysis was used to reveal the thermal transformation of sulfur species and the formation process of H2S. The results showed that kerogen decomposition and the corresponding products exert a strong influence on the transformation of organic sulfur and pyritic sulfur and, thus, on H2S formation. Before the peak hydrocarbon-generating stage ( |
| doi_str_mv | 10.1021/acs.energyfuels.0c04396 |
| format | Article |
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In our previous study, a series of artificial maturation experiments were conducted to simulate the hydrocarbon generation–retention–expulsion process. However, during the experiments, a large amount of hydrogen sulfide (H2S) was generated along with hydrocarbon products. Therefore, in this study, a combination of X-ray photoelectron spectroscopy, X-ray diffraction, and elemental analysis was used to reveal the thermal transformation of sulfur species and the formation process of H2S. The results showed that kerogen decomposition and the corresponding products exert a strong influence on the transformation of organic sulfur and pyritic sulfur and, thus, on H2S formation. Before the peak hydrocarbon-generating stage (<0.6% R o, 340 °C), the H2S yield was very low, primarily originating from organic sulfur in the kerogen. During the peak hydrocarbon generation and secondary cracking stage (0.6–1.24% R o, 340–400 °C), the H2S content showed an noticeable increase, and because the bulk atomic Sorg/C ratio remained relatively constant, the main source of H2S changed from organic sulfur to inorganic sulfur. Kerogen decomposition, pyrite decomposition, and thermochemical sulfate reduction (TSR) reactions contributed to H2S formation, whereas secondary pyrite formation consumed H2S. When the hydrocarbon generation potential of kerogen was almost exhausted, H2S exhibited an abnormally sharp increase, and little or no secondary pyrite was formed. The sulfur generated by pyrite decomposition partly formed H2S and partly incorporated into the organic matrix of kerogen. Hydrogen radicals generated by kerogen decomposition and secondary oil cracking are proposed as the controlling factor in the initial pyrite decomposition of the Chang 7 shale under the present pyrolysis experimental conditions.</description><identifier>ISSN: 0887-0624</identifier><identifier>EISSN: 1520-5029</identifier><identifier>DOI: 10.1021/acs.energyfuels.0c04396</identifier><language>eng</language><publisher>WASHINGTON: American Chemical Society</publisher><subject>Energy & Fuels ; Engineering ; Engineering, Chemical ; Fossil Fuels ; Science & Technology ; Technology</subject><ispartof>Energy & fuels, 2021-05, Vol.35 (9), p.7778-7786</ispartof><rights>2021 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>true</woscitedreferencessubscribed><woscitedreferencescount>4</woscitedreferencescount><woscitedreferencesoriginalsourcerecordid>wos000648878900051</woscitedreferencesoriginalsourcerecordid><citedby>FETCH-LOGICAL-a301t-f47a495d0aa7992177f777e3134b6dd3d49c5f8eea66f0a40b1429f9b76a321b3</citedby><cites>FETCH-LOGICAL-a301t-f47a495d0aa7992177f777e3134b6dd3d49c5f8eea66f0a40b1429f9b76a321b3</cites><orcidid>0000-0002-0044-5785 ; 0000-0003-2313-1516</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.energyfuels.0c04396$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.energyfuels.0c04396$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>315,782,786,2767,27083,27931,27932,39265,56745,56795</link.rule.ids></links><search><creatorcontrib>Ma, Weijiao</creatorcontrib><creatorcontrib>Hou, Lianhua</creatorcontrib><creatorcontrib>Luo, Xia</creatorcontrib><creatorcontrib>Liu, Jinzhong</creatorcontrib><creatorcontrib>Han, Wenxue</creatorcontrib><title>Thermal Transformation of Sulfur Species and Hydrogen Sulfide Formation in High-Pyrite-Containing Lacustrine Type-II Shale during Semiopen Pyrolysis</title><title>Energy & fuels</title><addtitle>ENERG FUEL</addtitle><addtitle>Energy Fuels</addtitle><description>The shale of the seventh member of the Triassic Yanchang Formation in the Ordos Basin (abbreviated as Chang 7 shale) is the most prospective shale for in situ conversion process. In our previous study, a series of artificial maturation experiments were conducted to simulate the hydrocarbon generation–retention–expulsion process. However, during the experiments, a large amount of hydrogen sulfide (H2S) was generated along with hydrocarbon products. Therefore, in this study, a combination of X-ray photoelectron spectroscopy, X-ray diffraction, and elemental analysis was used to reveal the thermal transformation of sulfur species and the formation process of H2S. The results showed that kerogen decomposition and the corresponding products exert a strong influence on the transformation of organic sulfur and pyritic sulfur and, thus, on H2S formation. Before the peak hydrocarbon-generating stage (<0.6% R o, 340 °C), the H2S yield was very low, primarily originating from organic sulfur in the kerogen. During the peak hydrocarbon generation and secondary cracking stage (0.6–1.24% R o, 340–400 °C), the H2S content showed an noticeable increase, and because the bulk atomic Sorg/C ratio remained relatively constant, the main source of H2S changed from organic sulfur to inorganic sulfur. Kerogen decomposition, pyrite decomposition, and thermochemical sulfate reduction (TSR) reactions contributed to H2S formation, whereas secondary pyrite formation consumed H2S. When the hydrocarbon generation potential of kerogen was almost exhausted, H2S exhibited an abnormally sharp increase, and little or no secondary pyrite was formed. The sulfur generated by pyrite decomposition partly formed H2S and partly incorporated into the organic matrix of kerogen. Hydrogen radicals generated by kerogen decomposition and secondary oil cracking are proposed as the controlling factor in the initial pyrite decomposition of the Chang 7 shale under the present pyrolysis experimental conditions.</description><subject>Energy & Fuels</subject><subject>Engineering</subject><subject>Engineering, Chemical</subject><subject>Fossil Fuels</subject><subject>Science & Technology</subject><subject>Technology</subject><issn>0887-0624</issn><issn>1520-5029</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><sourceid>HGBXW</sourceid><recordid>eNqNkF1LwzAUhoMoOD9-g7mXzqRJm-ZSirrBQGHzuqTtyZbRJSNpkf4Pf7CZG-KdXp0D5zwvLw9Cd5RMKUnpg2rCFCz49agH6MKUNIQzmZ-hCc1SkmQkledoQopCJCRP-SW6CmFLCMlZkU3Q52oDfqc6vPLKBu3i3htnsdN4OXR68Hi5h8ZAwMq2eDa23q3Bft9MC_j5BzAWz8x6k7yN3vSQlM72ylhj13ihmiH03ljAq3EPyXyOlxvVAW4Hf7gvYWfcPoZG1HVjMOEGXWjVBbg9zWv0_vy0KmfJ4vVlXj4uEsUI7RPNheIya4lSQsqUCqGFEMAo43Xetqzlssl0AaDyXBPFSU15KrWsRa5YSmt2jcQxt_EuBA-62nuzU36sKKkOcqsot_oltzrJjeT9kfyA2ukQBdkGfuiDXR6FFzJuGY3fxf-_S9N_Gy3dYPuIsiN6aLJ1g7dRyJ_1vgBDvqic</recordid><startdate>20210506</startdate><enddate>20210506</enddate><creator>Ma, Weijiao</creator><creator>Hou, Lianhua</creator><creator>Luo, Xia</creator><creator>Liu, Jinzhong</creator><creator>Han, Wenxue</creator><general>American Chemical Society</general><general>Amer Chemical Soc</general><scope>BLEPL</scope><scope>DTL</scope><scope>HGBXW</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-0044-5785</orcidid><orcidid>https://orcid.org/0000-0003-2313-1516</orcidid></search><sort><creationdate>20210506</creationdate><title>Thermal Transformation of Sulfur Species and Hydrogen Sulfide Formation in High-Pyrite-Containing Lacustrine Type-II Shale during Semiopen Pyrolysis</title><author>Ma, Weijiao ; Hou, Lianhua ; Luo, Xia ; Liu, Jinzhong ; Han, Wenxue</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a301t-f47a495d0aa7992177f777e3134b6dd3d49c5f8eea66f0a40b1429f9b76a321b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Energy & Fuels</topic><topic>Engineering</topic><topic>Engineering, Chemical</topic><topic>Fossil Fuels</topic><topic>Science & Technology</topic><topic>Technology</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ma, Weijiao</creatorcontrib><creatorcontrib>Hou, Lianhua</creatorcontrib><creatorcontrib>Luo, Xia</creatorcontrib><creatorcontrib>Liu, Jinzhong</creatorcontrib><creatorcontrib>Han, Wenxue</creatorcontrib><collection>Web of Science Core Collection</collection><collection>Science Citation Index Expanded</collection><collection>Web of Science - Science Citation Index Expanded - 2021</collection><collection>CrossRef</collection><jtitle>Energy & fuels</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ma, Weijiao</au><au>Hou, Lianhua</au><au>Luo, Xia</au><au>Liu, Jinzhong</au><au>Han, Wenxue</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Thermal Transformation of Sulfur Species and Hydrogen Sulfide Formation in High-Pyrite-Containing Lacustrine Type-II Shale during Semiopen Pyrolysis</atitle><jtitle>Energy & fuels</jtitle><stitle>ENERG FUEL</stitle><addtitle>Energy Fuels</addtitle><date>2021-05-06</date><risdate>2021</risdate><volume>35</volume><issue>9</issue><spage>7778</spage><epage>7786</epage><pages>7778-7786</pages><issn>0887-0624</issn><eissn>1520-5029</eissn><abstract>The shale of the seventh member of the Triassic Yanchang Formation in the Ordos Basin (abbreviated as Chang 7 shale) is the most prospective shale for in situ conversion process. In our previous study, a series of artificial maturation experiments were conducted to simulate the hydrocarbon generation–retention–expulsion process. However, during the experiments, a large amount of hydrogen sulfide (H2S) was generated along with hydrocarbon products. Therefore, in this study, a combination of X-ray photoelectron spectroscopy, X-ray diffraction, and elemental analysis was used to reveal the thermal transformation of sulfur species and the formation process of H2S. The results showed that kerogen decomposition and the corresponding products exert a strong influence on the transformation of organic sulfur and pyritic sulfur and, thus, on H2S formation. Before the peak hydrocarbon-generating stage (<0.6% R o, 340 °C), the H2S yield was very low, primarily originating from organic sulfur in the kerogen. During the peak hydrocarbon generation and secondary cracking stage (0.6–1.24% R o, 340–400 °C), the H2S content showed an noticeable increase, and because the bulk atomic Sorg/C ratio remained relatively constant, the main source of H2S changed from organic sulfur to inorganic sulfur. Kerogen decomposition, pyrite decomposition, and thermochemical sulfate reduction (TSR) reactions contributed to H2S formation, whereas secondary pyrite formation consumed H2S. When the hydrocarbon generation potential of kerogen was almost exhausted, H2S exhibited an abnormally sharp increase, and little or no secondary pyrite was formed. The sulfur generated by pyrite decomposition partly formed H2S and partly incorporated into the organic matrix of kerogen. Hydrogen radicals generated by kerogen decomposition and secondary oil cracking are proposed as the controlling factor in the initial pyrite decomposition of the Chang 7 shale under the present pyrolysis experimental conditions.</abstract><cop>WASHINGTON</cop><pub>American Chemical Society</pub><doi>10.1021/acs.energyfuels.0c04396</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0002-0044-5785</orcidid><orcidid>https://orcid.org/0000-0003-2313-1516</orcidid></addata></record> |
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| subjects | Energy & Fuels Engineering Engineering, Chemical Fossil Fuels Science & Technology Technology |
| title | Thermal Transformation of Sulfur Species and Hydrogen Sulfide Formation in High-Pyrite-Containing Lacustrine Type-II Shale during Semiopen Pyrolysis |
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