Encapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate

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	Encapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate
	Zhu, JL ; Du, SY ; Yu, XH ; Zhang, JZ ; Xu, HW ; Vogel, SC ; Germann, TC ; Francisco, JS ; Izumi, F ; Momma, K ; Kawamura, Y ; Jin, CQ ; Zhao, YS
刊名	NATURE COMMUNICATIONS
	2014
卷号	5
ISSN号	2041-1723
通讯作者	Yu, XH (reprint author), Los Alamos Natl Lab, LANSCE, POB 1663, Los Alamos, NM 87545 USA.
中文摘要	Carbon monoxide clathrate hydrate is a potentially important constituent in the solar system. In contrast to the well-established relation between the size of gaseous molecule and hydrate structure, previous work showed that carbon monoxide molecules preferentially form structure-I rather than structure-II gas hydrate. Resolving this discrepancy is fundamentally important to understanding clathrate formation, structure stabilization and the role the dipole moment/molecular polarizability plays in these processes. Here we report the synthesis of structure-II carbon monoxide hydrate under moderate high-pressure/low-temperature conditions. We demonstrate that the relative stability between structure-I and structure-II hydrates is primarily determined by kinetically controlled cage filling and associated binding energies. Within hexakaidecahedral cage, molecular dynamic simulations of density distributions reveal eight low-energy wells forming a cubic geometry in favour of the occupancy of carbon monoxide molecules, suggesting that the carbon monoxide-water and carbon monoxide-carbon monoxide interactions with adjacent cages provide a significant source of stability for the structure-II clathrate framework.
资助信息	Los Alamos National Laboratory - Los Alamos National Security LLC under DOE [DE-AC52-06NA25396]; US Department of Energy's Office of Basic Energy Sciences; Institute of Physics, Chinese Academy of Sciences (IOPCAS) - CAS project [KJCX2-YW-W26, XDB07000000]; High Pressure Science and Engineering Center (HiPSEC), UNLV; National Nuclear Security Administration under the Stewardship Science Academic Alliances program through DOE Cooperative Agreement [DE-NA0001982]
语种	英语
公开日期	2015-04-14
内容类型	期刊论文
源URL	[http://ir.iphy.ac.cn/handle/311004/59385]
专题	物理研究所_物理所公开发表论文_物理所公开发表论文_期刊论文
推荐引用方式 GB/T 7714	Zhu, JL,Du, SY,Yu, XH,et al. Encapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate[J]. NATURE COMMUNICATIONS,2014,5.
APA	Zhu, JL.,Du, SY.,Yu, XH.,Zhang, JZ.,Xu, HW.,...&Zhao, YS.(2014).Encapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate.NATURE COMMUNICATIONS,5.
MLA	Zhu, JL,et al."Encapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate".NATURE COMMUNICATIONS 5(2014).