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
发表期刊GEOCHIMICA ET COSMOCHIMICA ACTA
卷号118页码:263-275
摘要Elemental 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.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1016/j.gca.2013.05.021
收录类别SCI
语种英语
关键词[WOS]DEEP CARBONATE RESERVOIRS ; VALLEY-TYPE DEPOSITS ; SICHUAN BASIN ; SIMULATION EXPERIMENTS ; SMACKOVER FORMATION ; BURIAL DIAGENESIS ; HYDROGEN-SULFIDE ; AQUEOUS SULFATE ; KHUFF FORMATION ; ORGANIC-MATTER
WOS类目Geochemistry & Geophysics
WOS记录号WOS:000324035800016
引用统计
被引频次:13[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.idsse.ac.cn/handle/183446/733
专题深海科学研究部_深海极端环境模拟研究实验室
作者单位1.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
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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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