Effects of ensembles on methane hydrate nucleation kinetics

doi:10.1039/c6cp02171a

GIEC OpenIR > 中国科学院广州能源研究所

	Effects of ensembles on methane hydrate nucleation kinetics
	Zhang, Zhengcai 1; Liu, Chan-Juan 2; Walsh, Matthew R.3; Guo, Guang-Jun 1
	2016-06-21
发表期刊	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷号	18 期号:23 页码:15602-15608
摘要	By performing molecular dynamics simulations to form a hydrate with a methane nano-bubble in liquid water at 250 K and 50 MPa, we report how different ensembles, such as the NPT, NVT, and NVE ensembles, affect the nucleation kinetics of the methane hydrate. The nucleation trajectories are monitored using the face-saturated incomplete cage analysis (FSICA) and the mutually coordinated guest (MCG) order parameter (OP). The nucleation rate and the critical nucleus are obtained using the mean first-passage time (MFPT) method based on the FS cages and the MCG-1 OPs, respectively. The fitting results of MFPT show that hydrate nucleation and growth are coupled together, consistent with the cage adsorption hypothesis which emphasizes that the cage adsorption of methane is a mechanism for both hydrate nucleation and growth. For the three different ensembles, the hydrate nucleation rate is quantitatively ordered as follows: NPT > NVT > NVE, while the sequence of hydrate crystallinity is exactly reversed. However, the largest size of the critical nucleus appears in the NVT ensemble, rather than in the NVE ensemble. These results are helpful for choosing a suitable ensemble when to study hydrate formation via computer simulations, and emphasize the importance of the order degree of the critical nucleus.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences
DOI	10.1039/c6cp02171a
研究领域[WOS]	Chemistry ; Physics
关键词[WOS]	MOLECULAR-DYNAMICS SIMULATIONS ; HOMOGENEOUS CRYSTAL NUCLEATION ; GAS HYDRATE ; AQUEOUS METHANE ; LIQUID WATER ; GROWTH ; MECHANISMS ; SIZE ; CRYSTALLIZATION ; SOLUBILITY
收录类别	SCI
语种	英语
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000378243000017
引用统计	被引频次：47[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/344007/11774
专题	中国科学院广州能源研究所
作者单位	1.Chinese Acad Sci, Inst Geol & Geophys, Key Lab Earth & Planetary Phys, Beijing 100029, Peoples R China 2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Gas Hydrate, Guangzhou 510640, Guangdong, Peoples R China 3.Chevron Energy Technol Co, Flow Assurance, 1400 Smith St, Houston, TX 77002 USA
推荐引用方式 GB/T 7714	Zhang, Zhengcai,Liu, Chan-Juan,Walsh, Matthew R.,et al. Effects of ensembles on methane hydrate nucleation kinetics[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2016,18(23):15602-15608.
APA	Zhang, Zhengcai,Liu, Chan-Juan,Walsh, Matthew R.,&Guo, Guang-Jun.(2016).Effects of ensembles on methane hydrate nucleation kinetics.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,18(23),15602-15608.
MLA	Zhang, Zhengcai,et al."Effects of ensembles on methane hydrate nucleation kinetics".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 18.23(2016):15602-15608.