Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates

doi:10.1021/acs.jpcc.6b07444

GIEC OpenIR > 中国科学院广州能源研究所

	Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates
	Zhou, Xuebing 1,2; Lin, Fuhua 1,2; Liang, Deqing1,2
	2016-11-17
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C
卷号	120 期号:45 页码:25668-25677
摘要	Swapping CH4 with CO2 in hydrocarbon hydrates is renowned as an eco-friendly method for potential energy production and climate change mitigation. To fully understand the CH4-CO2 replacement process, in situ Raman spectroscopy combined with long-term macroscopic measurements were carried out by putting CH4 hydrates into gaseous CO2 at temperatures ranging from 273.2 to 281.2 K. A kinetic model based on gas diffusion theory was modified. Results showed that the gas swapping process started with surface reaction followed by gas diffusion in hydrate phase. At hydrate surface, the average occupancy of CH4 decreased without dramatic fluctuations, suggesting that the replacements were not simply composed of a series of dissociation and reformation process. A rise in temperature was found to effectively increase the gas swapping rates and strengthen the gas diffusion in hydrate phase. In situ Raman results together with gas consumption data were fitted by the kinetic model. The calculated gas-hydrate interfacial area revealed the foamy nature of hydrates. Fitting parameters representing the gas diffusion coefficient were of the same order of magnitude as the water mobility in hydrate phase, which implied that the replacements were limited by the mobility of water molecules.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences ; Technology
DOI	10.1021/acs.jpcc.6b07444
研究领域[WOS]	Chemistry ; Science & Technology - Other Topics ; Materials Science
关键词[WOS]	NATURAL-GAS HYDRATE ; METHANE HYDRATE ; CARBON-DIOXIDE ; LIQUID CO2 ; IN-SITU ; RAMAN-SPECTROSCOPY ; CURRENT KNOWLEDGE ; PRESSURIZED CO2 ; CH4 HYDRATE ; REPLACEMENT
收录类别	SCI
语种	英语
项目资助者	National Natural Science Foundation of China(51176192 ; CAS Program(KGZD-EW-301) ; CAS(2015A-4813) ; Scientific cooperative project by CNPC ; 51376182)
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000388429100004
引用统计	被引频次：27[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.giec.ac.cn/handle/344007/13978
专题	中国科学院广州能源研究所
作者单位	1.Chinese Acad Sci, Key Lab Gas Hydrate, Guangzhou Inst Energy Convers, Guangzhou 510640, Guangdong, Peoples R China 2.Guangdong Key Lab New & Renewable Energy Res & De, Guangzhou 510640, Guangdong, Peoples R China
推荐引用方式 GB/T 7714	Zhou, Xuebing,Lin, Fuhua,Liang, Deqing. Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2016,120(45):25668-25677.
APA	Zhou, Xuebing,Lin, Fuhua,&Liang, Deqing.(2016).Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates.JOURNAL OF PHYSICAL CHEMISTRY C,120(45),25668-25677.
MLA	Zhou, Xuebing,et al."Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates".JOURNAL OF PHYSICAL CHEMISTRY C 120.45(2016):25668-25677.