Atomistic Simulation of Nafion Membrane. 2. Dynamics of Water Molecules and Hydronium Ions

作者：Ram Devanathan, Arun Venkatnathan, Michel Dupuis · 发表于：The Journal of Physical Chemistry B · 年份：2007 · DOI：10.1021/jp0761057 · 被引用次数：173 · 研究领域：Fuel Cells and Related Materials、Advanced battery technologies research、Advanced Battery Technologies Research

We have performed a detailed and comprehensive analysis of the dynamics of water molecules and hydronium ions in hydrated Nafion using classical molecular dynamics simulations with the DREIDING force field. In addition to calculating diffusion coefficients as a function of hydration level, we have also determined mean residence time of H(2)O molecules and H(3)O(+) ions in the first solvation shell of SO(3)(-) groups. The diffusion coefficient of H(2)O molecules increases with increasing hydration level and is in good agreement with experiment. The mean residence time of H(2)O molecules decreases with increasing membrane hydration from 1 ns at a low hydration level to 75 ps at the highest hydration level studied. These dynamical changes are related to the changes in membrane nanostructure reported in the first part of this work. Our results provide insights into slow proton dynamics observed in neutron scattering experiments and are consistent with the Gebel model of Nafion structure.