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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
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY C
Volume120Issue:45Pages:25668-25677
AbstractSwapping 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.
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
DOI10.1021/acs.jpcc.6b07444
WOS Subject ExtendedChemistry ; Science & Technology - Other Topics ; Materials Science
WOS KeywordNATURAL-GAS HYDRATE ; METHANE HYDRATE ; CARBON-DIOXIDE ; LIQUID CO2 ; IN-SITU ; RAMAN-SPECTROSCOPY ; CURRENT KNOWLEDGE ; PRESSURIZED CO2 ; CH4 HYDRATE ; REPLACEMENT
Indexed BySCI
Language英语
Funding OrganizationNational Natural Science Foundation of China(51176192 ; CAS Program(KGZD-EW-301) ; CAS(2015A-4813) ; Scientific cooperative project by CNPC ; 51376182)
WOS SubjectChemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000388429100004
Citation statistics
Document Type期刊论文
Identifierhttp://ir.giec.ac.cn/handle/344007/13978
Collection中国科学院广州能源研究所
Affiliation1.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
Recommended Citation
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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