Water Diffusion in Amorphous Hydrophilic Systems: A Stop and Go Process

被引:43
作者
Kulasinski, Karol [1 ,2 ]
Guyer, Robert [3 ,4 ]
Derome, Dominique [2 ]
Carmeliet, Jan [1 ,2 ]
机构
[1] ETH, Swiss Fed Univ Technol, Chair Bldg Phys, CH-8093 Zurich, Switzerland
[2] Swiss Fed Labs Mat Sci & Technol Empa, Lab Multiscale Studies Bldg Phys, CH-8600 Dubendorf, Switzerland
[3] Los Alamos Natl Lab, Solid Earth Geophys Grp, Los Alamos, NM 87545 USA
[4] Univ Nevada, Dept Phys, Reno, NV 89557 USA
关键词
GROMOS FORCE-FIELD; SYNCHROTRON X-RAY; MOLECULAR-DYNAMICS; BOUND WATER; CELLULOSE; WOOD; ADSORPTION; SPRUCE; MODEL; CRYSTALLINE;
D O I
10.1021/acs.langmuir.5b03122
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The diffusion of H2O in three amorphous polymer H2O systems is studied as a function of H2O content using molecular dynamics. A picture of H2O molecule motion comprising alternating steps of being bound at an adsorption site ("stop") and moving ("go") emerges. This picture is made quantitative. The bound time, frequency of stop go steps, and tortuosity all decrease with H2O content. Fourier analysis of particle motion during bound time segments provides a measure of an attempt frequency that is connected quantitatively to the bound time and an activation energy of a hydrogen bond. For increasing H2O content, the polymer H2O systems swell, leading to an increase in the diffusion coefficient and porosity and a decrease in activation energy.
引用
收藏
页码:10843 / 10849
页数:7
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