Force-based method to determine the potential dependence in electrochemical barriers
- 1. CatTheory, Department of Physics, Technical University of Denmark, 2800 Kgs. Lyngby, Denmark
- 2. SUNCAT Center for Interface Science and Catalysis
- 3. Department of Chemical and Biomolecular Engineering, University of California, Berkeley
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Description
Determining ab-initio potential dependent energetics are critical to investigating 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 which 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 super-cell sizes and proton concentrations for a range of electrochemical reactions. This record contains output files from all the DFT calculations needed to reproduce the figures in the manuscript.
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Preprint Vijay S, Kastlunger G, Gauthier JA, Patel A, Chan K. Force-based method to determine the potential dependence in electrochemical barriers. ChemRxiv. Cambridge: Cambridge Open Engage; 2022, doi: 10.26434/chemrxiv-2022-lm0f7