Disproportionation and thermochemical sulfate reduction reactions in;S-H2O-CH4 and S-D2O-CH4 systems from 200 to 340 degrees C at elevated;pressures

doi:10.1016/j.gca.2013.05.021

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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, Shunda 1; Chou, I-Ming ; Burruss, Robert C.; Wang, Xiaolin 5,6; Li, Jiankang
刊名	GEOCHIMICA ET COSMOCHIMICA ACTA
	2013
卷号	118 页码:263-275
ISSN号	0016-7037
DOI	10.1016/j.gca.2013.05.021
英文摘要	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.
学科主题	地球化学
WOS关键词	DEEP CARBONATE RESERVOIRS ; VALLEY-TYPE DEPOSITS ; SICHUAN BASIN ; SIMULATION EXPERIMENTS ; SMACKOVER FORMATION ; BURIAL DIAGENESIS ; HYDROGEN-SULFIDE ; AQUEOUS SULFATE ; KHUFF FORMATION ; ORGANIC-MATTER
WOS研究方向	Geochemistry & Geophysics
语种	英语
出版者	PERGAMON-ELSEVIER SCIENCE LTD
WOS记录号	WOS:000324035800016
内容类型	期刊论文
源URL	[http://119.78.100.197/handle/2HKVOGP0/40011]
专题	中国地质科学院矿产资源研究所
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.Burruss, Robert C.] 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.
推荐引用方式 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.