Molecular Mechanisms of Gas Diffusion in CO2 Hydrates

doi:10.1021/acs.jpcc.6b03111

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	Molecular Mechanisms of Gas Diffusion in CO2 Hydrates
	Liang, Shuai 1; Liang, Deqing1 ; Wu, Nengyou2,3 ; Yi, Lizhi 1; Hu, Gaowei 2,3
	2016-08-04
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C
卷号	120 期号:30 页码:16298-16304
摘要	Gas diffusion is considered a rate-limiting step in the formation of gas hydrates, yet its molecular 'mechanisms remain unclear. In this work, we present the molecular mechanisms of the CO2 cage-to-cage transport in gas hydrates, as directly observed from molecular dynamics simulations performed at elevated temperatures. We found that at least one water vacancy is required for the CO2 molecules to pass through five-membered water rings, while only the distortion of the local ring structure is required for the CO2 molecules to pass through the six-membered water rings. We used the transition-state theory to estimate the relevant kinetic parameters associated with the CO2 diffusion in gas hydrates. The calculated free energy of activation is about 44 +/- 6 kJ/mol, and the diffusion coefficient is in the range of 1.0 X 10-(16) similar to 2.0 x 10(-14) m(2)/s, for the CO2 diffusion at 270 K, in close agreement with previous experiments. This work suggests that the presence of empty cages is crucial for the CO2 cage-to-cage transport in gas, hydrates.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences ; Technology
DOI	10.1021/acs.jpcc.6b03111
研究领域[WOS]	Chemistry ; Science & Technology - Other Topics ; Materials Science
关键词[WOS]	CARBON-DIOXIDE HYDRATE ; CLATHRATE HYDRATE ; METHANE HYDRATE ; IN-SITU ; DYNAMICS SIMULATIONS ; WATER ; REPLACEMENT ; HYDROGEN ; GROWTH ; ENERGY
收录类别	SCI
语种	英语
项目资助者	National Natural Science Foundation of China(41473063 ; CAS Program(KGZD-EW-301) ; 41474119)
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000381236100004
引用统计	被引频次：44[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/344007/11837
专题	中国科学院广州能源研究所
作者单位	1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Gas Hydrate, Guangdong Key Lab New & Renewable Energy Res & De, Guangzhou 510640, Guangdong, Peoples R China 2.Qingdao Natl Lab Marine Sci & Technol, Lab Marine Mineral Resources, Qingdao 266071, Peoples R China 3.Qingdao Inst Marine Geol, Minist Land & Resources, Key Lab Gas Hydrate, Qingdao 266071, Peoples R China
第一作者单位	中国科学院广州能源研究所
推荐引用方式 GB/T 7714	Liang, Shuai,Liang, Deqing,Wu, Nengyou,et al. Molecular Mechanisms of Gas Diffusion in CO2 Hydrates[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2016,120(30):16298-16304.
APA	Liang, Shuai,Liang, Deqing,Wu, Nengyou,Yi, Lizhi,&Hu, Gaowei.(2016).Molecular Mechanisms of Gas Diffusion in CO2 Hydrates.JOURNAL OF PHYSICAL CHEMISTRY C,120(30),16298-16304.
MLA	Liang, Shuai,et al."Molecular Mechanisms of Gas Diffusion in CO2 Hydrates".JOURNAL OF PHYSICAL CHEMISTRY C 120.30(2016):16298-16304.