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Multiscale Analysis on CH4-CO2 Swapping Phenomenon Occurred in Hydrates
Zhou, Xuebing1,2; Lin, Fuhua1,2; 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
资助者National Natural Science Foundation of China(51176192 ; CAS Program(KGZD-EW-301) ; CAS(2015A-4813) ; Scientific cooperative project by CNPC ; 51376182) ; National Natural Science Foundation of China(51176192 ; CAS Program(KGZD-EW-301) ; CAS(2015A-4813) ; Scientific cooperative project by CNPC ; 51376182)
DOI10.1021/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
资助者National Natural Science Foundation of China(51176192 ; CAS Program(KGZD-EW-301) ; CAS(2015A-4813) ; Scientific cooperative project by CNPC ; 51376182) ; 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:4[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
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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.
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