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Disproportionation and thermochemical sulfate reduction reactions in S-H2O-CH4 and S-D2O-CH4 systems from 200 to 340 degrees C at elevated pressures
Yuan, Shunda1,2,3; Chou, I-Ming3,4; Burruss, Robert C.5; Wang, Xiaolin6,7; Li, Jiankang1
2013-10-01
Source PublicationGEOCHIMICA ET COSMOCHIMICA ACTA
Volume118Pages:263-275
AbstractElemental sulfur, as a transient intermediate compound, by-product, or catalyst, plays significant roles in thermochemical sulfate reduction (TSR) reactions. However, the mechanisms of the reactions in S-H2O-hydrocarbons systems are not clear. To improve our understanding of reaction mechanisms, we conducted a series of experiments between 200 and 340 degrees C for S-H2O-CH4, S-D2O-CH4, and S-CH4-1m ZnBr2 systems in fused silica capillary capsules (FSCCs). After a heating period ranging from 24 to 2160 h (hrs), the quenched samples were analyzed by Raman spectroscopy. Combined with the in situ Raman spectra collected at high temperatures and pressures in the S-H2O and S-H2O-CH4 systems, our results showed that (1) the disproportionation of sulfur in the S-H2O-CH4 system occurred at temperatures above 200 degrees C and produced H2S, SO42-, and possibly trace amount of HSO4-; (2) sulfate (and bisulfate), in the presence of sulfur, can be reduced by methane between 250 and 340 degrees C to produce CO2 and H2S, and these TSR temperatures are much closer to those of the natural system (<200 degrees C) than those of any previous experiments; (3) the disproportionation and TSR reactions in the S-H2O-CH4 system may take place simultaneously, with TSR being favored at higher temperatures; and, (4) in the system S-D2O-CH4, both TSR and the competitive disproportionation reactions occurred simultaneously at temperatures above 300 degrees C, but these reactions were very slow at lower temperatures. Our observation of methane reaction at 250 degrees C in a laboratory time scale suggests that, on a geologic time scale, methane may be destroyed by TSR reactions at temperatures >200 degrees C that can be reached by deep drilling for hydrocarbon resources. (C) 2013 Elsevier Ltd. All rights reserved.
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1016/j.gca.2013.05.021
Indexed BySCI
Language英语
WOS KeywordDEEP CARBONATE RESERVOIRS ; VALLEY-TYPE DEPOSITS ; SICHUAN BASIN ; SIMULATION EXPERIMENTS ; SMACKOVER FORMATION ; BURIAL DIAGENESIS ; HYDROGEN-SULFIDE ; AQUEOUS SULFATE ; KHUFF FORMATION ; ORGANIC-MATTER
WOS SubjectGeochemistry & Geophysics
WOS IDWOS:000324035800016
Citation statistics
Cited Times:15[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.idsse.ac.cn/handle/183446/733
Collection深海科学研究部_深海极端环境模拟研究实验室
Affiliation1.CAGS, MLR Key Lab Metallogeny & Mineral Assessment, Inst Mineral Resources, Beijing 100037, Peoples R China
2.Chinese Acad Sci, Inst Geochem, State Key Lab Ore Deposit Geochem, Guiyang 550002, Peoples R China
3.US Geol Survey, Natl Ctr 954, Reston, VA 20192 USA
4.Chinese Acad Sci, Sanya Inst Deep Sea Sci & Engn, Lab Expt Study Deep Sea Extreme Condit, Sanya 572000, Peoples R China
5.US Geol Survey, Natl Ctr 956, Reston, VA 20192 USA
6.Nanjing Univ, State Key Lab Mineral Deposits Res, Sch Earth Sci & Engn, Nanjing 210093, Jiangsu, Peoples R China
7.Nanjing Univ, Inst Energy Sci, Sch Earth Sci & Engn, Nanjing 210093, Jiangsu, Peoples R China
Recommended Citation
GB/T 7714
Yuan, Shunda,Chou, I-Ming,Burruss, Robert C.,et al. Disproportionation and thermochemical sulfate reduction reactions in S-H2O-CH4 and S-D2O-CH4 systems from 200 to 340 degrees C at elevated pressures[J]. GEOCHIMICA ET COSMOCHIMICA ACTA,2013,118:263-275.
APA Yuan, Shunda,Chou, I-Ming,Burruss, Robert C.,Wang, Xiaolin,&Li, Jiankang.(2013).Disproportionation and thermochemical sulfate reduction reactions in S-H2O-CH4 and S-D2O-CH4 systems from 200 to 340 degrees C at elevated pressures.GEOCHIMICA ET COSMOCHIMICA ACTA,118,263-275.
MLA Yuan, Shunda,et al."Disproportionation and thermochemical sulfate reduction reactions in S-H2O-CH4 and S-D2O-CH4 systems from 200 to 340 degrees C at elevated pressures".GEOCHIMICA ET COSMOCHIMICA ACTA 118(2013):263-275.
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