Nanoscale heterogeneity at the aqueous electrolyte–electrode interface
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Willard_Nanoscale heterogeneity.pdf
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3.52 MB
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Checksum (MD5)
2f926d8139128a55f9a2ec2f46c606e2
Author(s)
Limmer, David T.
Willard, Adam P.
Date Issued
November 2014
Journal
Chemical Physics Letters
Publisher
Elsevier
Citation
Limmer, David T., and Adam P. Willard. “Nanoscale Heterogeneity at the Aqueous Electrolyte–electrode Interface.” Chemical Physics Letters 620 (2015): 144–150.
Version
Original manuscript
Abstract
Using molecular dynamics simulations, we reveal emergent properties of hydrated electrode interfaces that while molecular in origin are integral to the behavior of the system across long times scales and large length scales. Specifically, we describe the impact of a disordered and slowly evolving adsorbed layer of water on the molecular structure and dynamics of the electrolyte solution adjacent to it. Generically, we find that densities and mobilities of both water and dissolved ions are spatially heterogeneous in the plane parallel to the electrode over nanosecond timescales. These and other recent results are analyzed in the context of available experimental literature from surface science and electrochemistry. We speculate on the implications of this emerging microscopic picture on the catalytic proficiency of hydrated electrodes, offering a new direction for study in heterogeneous catalysis at the nanoscale.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution-NonCommercial-NoDerivs License
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1016/j.cplett.2014.11.013
