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Reaction pathway, mechanism and kinetics of thermochemical sulfate reduction: insights from in situ Raman spectroscopic observations at elevated temperatures and pressures

文献类型：期刊论文

作者Wan, Qian3; Wang, Xiaolin2,3; Hu, Wenxuan2,3; Wan, Ye1; Chou, I. -Ming1
刊名GEOCHIMICA ET COSMOCHIMICA ACTA
出版日期2024-09-15
卷号381页码:25-42
关键词Thermochemical sulfate reduction Reaction pathway Sulfur speciation Kinetics In situ observation MVT deposits
ISSN号0016-7037
DOI10.1016/j.gca.2024.07.027
英文摘要In Earth's crust, thermochemical sulfate reduction (TSR) is a common organic-inorganic interaction, which is in close association with the carbon cycle in sedimentary basins and metal sulfide precipitation in Mississippi Valley-type deposits. However, the reaction pathway and mechanism of TSR need further investigation, mainly due to the complex sulfur species involved in this reaction. Here we applied in situ Raman spectroscopy to disclose the stepwise transformation from sulfate to sulfide and the reaction kinetics in the CH4-Na2SO4/MgSO4/H2SO4-H2O systems at elevated temperatures and pressures. Our results indicate that sulfate is transformed to H2S through a series of reduction and disproportionation reactions. Once dissolved H2S reaches a certain concentration, it reacts with sulfate to form intermediate valence sulfur species (S-0 and S-3(-)), which quickly oxidize methane to generate CO2 and H2S. The formation of S-3(-) and S-0 is responsible for the autocatalytic effect in TSR. The sulfur speciation significantly affects the reaction kinetics, which could be divided into three stages based on the in situ observations. Extrapolated kinetic data show that TSR could proceed fast under the catalysis of H2S, and the half-life of methane is similar to 7.10 million years at 200 degrees C. Subsequent numerical modeling strongly supports that in situ sulfate reduction could provide sufficient reduced sulfur for the formation of giant Mississippi Valley-type deposits, thus serving as an efficient mineralizing mechanism.
WOS关键词VALLEY-TYPE DEPOSITS ; ORGANIC-INORGANIC INTERACTIONS ; TRIASSIC FEIXIANGUAN FORMATION ; CARBONATE GAS-RESERVOIRS ; SULFUR ISOTOPE-EXCHANGE ; EAST SICHUAN BASIN ; ELEMENTAL SULFUR ; PRECIPITATION MECHANISMS ; HYDROTHERMAL FLUIDS ; SMACKOVER FORMATION
资助项目National Key Research and Development Program of China[2022YFF0800403] ; National Natural Science Foundation of China[42173038] ; Research Funds for the Frontiers Science Center for Critical Earth Material Cycling (Nanjing University) ; Fundamental Research Funds for the Central Universities ; PetroChina Foundation Projects for Basic Scientific Research and Strategic Technology Reserves[2023D-5008-02]
WOS研究方向Geochemistry & Geophysics
语种英语
WOS记录号WOS:001288042400001
出版者PERGAMON-ELSEVIER SCIENCE LTD
资助机构National Key Research and Development Program of China ; National Natural Science Foundation of China ; Research Funds for the Frontiers Science Center for Critical Earth Material Cycling (Nanjing University) ; Fundamental Research Funds for the Central Universities ; PetroChina Foundation Projects for Basic Scientific Research and Strategic Technology Reserves
源URL[http://ir.idsse.ac.cn/handle/183446/11469]  
专题深海科学研究部_深海极端环境模拟研究实验室
通讯作者Wang, Xiaolin
作者单位1.Chinese Acad Sci, Inst Deep Sea Sci & Engn, Sanya 572000, Hainan, Peoples R China
2.Nanjing Univ, Frontiers Sci Ctr Crit Earth Mat Cycling, Nanjing 210023, Jiangsu, Peoples R China
3.Nanjing Univ, Sch Earth Sci & Engn, State Key Lab Mineral Deposits Res, Nanjing 210023, Jiangsu, Peoples R China
推荐引用方式
GB/T 7714		 Wan, Qian,Wang, Xiaolin,Hu, Wenxuan,et al. Reaction pathway, mechanism and kinetics of thermochemical sulfate reduction: insights from in situ Raman spectroscopic observations at elevated temperatures and pressures[J]. GEOCHIMICA ET COSMOCHIMICA ACTA,2024,381:25-42.
APA Wan, Qian,Wang, Xiaolin,Hu, Wenxuan,Wan, Ye,&Chou, I. -Ming.(2024).Reaction pathway, mechanism and kinetics of thermochemical sulfate reduction: insights from in situ Raman spectroscopic observations at elevated temperatures and pressures.GEOCHIMICA ET COSMOCHIMICA ACTA,381,25-42.
MLA Wan, Qian,et al."Reaction pathway, mechanism and kinetics of thermochemical sulfate reduction: insights from in situ Raman spectroscopic observations at elevated temperatures and pressures".GEOCHIMICA ET COSMOCHIMICA ACTA 381(2024):25-42.

入库方式： OAI收割

来源：深海科学与工程研究所

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