期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 115, 期 43, 页码 21241-21248出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp206483q
关键词
-
资金
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-05ER46242]
- CSM Hydrate Consortium
- NSF [CBET-0933856]
- Taiwan NSC
- NSF
- National Renewable Energy Laboratory
- Office of Energy Efficiency and Renewable Energy of the United States Department of Energy [DE-AC36-08GO28308]
Methane hydrate nucleation rates are reported from over 200 mu s of molecular dynamics simulations across a range of thermodynamic conditions and varying degrees of methane-water interfacial curvature. Calculated nucleation rates increase with aqueous phase methane concentration (X-CH4), consistent with experimental results. The effect of interfacial curvature on X-CH4 is quantified, with dissolved methane concentration increasing with the degree of curvature (i.e., the number of dimensions in which curvature exists). Nucleation rates are reported for system sizes of 3456 and 13 824 molecules (H2O + CH4). Among the smaller simulation systems (which comprise the majority of the data), the calculated hydrate nucleation rates follow the same trend when plotted against X-CH4 regardless of whether the predominant contribution to the effective system pressure is the simulation barostat or the methane-water interfacial curvature (Young-Laplace pressure). The incipient hydrate nuclei are destabilized in the immediate vicinity (similar to 1 n.m) of the methane-water interface, and the calculated nucleation rates for the larger simulation systems (in which the incipient hydrate solids are less affected by interfacial destabilization) fall above the trend observed in the smaller systems.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据