Journal article
Force-Based Method to Determine the Potential Dependence in Electrochemical Barriers
Determining ab initio potential-dependent energetics is critical to the investigation of mechanisms for electrochemical reactions. While methodology for evaluating reaction thermodynamics is established, simulation techniques for the corresponding kinetics is still a major challenge owing to a lack of potential control, finite cell size effects, or computational expense.
In this work, we develop a model that allows for computing electrochemical activation energies from just a handful of density functional theory (DFT) calculations. The sole input into the model are the atom-centered forces obtained from DFT calculations performed on a homogeneous grid composed of varying field strengths.
We show that the activation energies as a function of the potential obtained from our model are consistent for different supercell sizes and proton concentrations for a range of electrochemical reactions.
Language: | English |
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Publisher: | American Chemical Society |
Year: | 2022 |
Pages: | 5719-5725 |
ISSN: | 19487185 |
Types: | Journal article |
DOI: | 10.1021/acs.jpclett.2c01367 |
ORCIDs: | 0000-0001-8242-0161 , Kastlunger, Georg , 0000-0001-9542-0988 , 0000-0002-0590-7619 and Chan, Karen |