Proton Transport under External Applied Voltage
Z Cao and R Kumar and YX Peng and GA Voth, JOURNAL OF PHYSICAL CHEMISTRY B, 118, 8090-8098 (2014).
DOI: 10.1021/jp501130m
Proton transport through an electrolyte layer between platinum electrodes under a range of applied voltages is explored using reactive molecular dynamics simulation. The proton transport process is decomposed into vehicular and Grotthuss hopping components, and the two mechanisms and their correlation are investigated as a function of applied voltage. At higher applied voltages, the effect of the hopping mechanism is much larger as compared with the vehicular mechanism. As the voltage is increased, the net correlation between the two mechanisms goes from negative to positive, and both the hopping frequency as well as the number of consecutive forward hops increases. This behavior results in a larger total diffusion constant at higher values of the voltage. The behavior of the hydrated excess proton is therefore substantially different under an applied external voltage than in the normal bulk water environment.
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