Force-Based Method to Determine the Potential Dependence in Electrochemical Barriers
- Sudarshan Vijay*Sudarshan Vijay*[email protected]CatTheory, Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby, DenmarkMore by Sudarshan Vijay
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- Georg KastlungerGeorg KastlungerCatTheory, Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby, DenmarkMore by Georg Kastlunger
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- Joseph A. GauthierJoseph A. GauthierChemical Sciences Division, Lawrence Berkeley National Laboratory, 94720 Berkeley, California, United StatesDepartment of Chemical and Biomolecular Engineering, University of California, 94720 Berkeley, California, United StatesMore by Joseph A. Gauthier
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- Anjli PatelAnjli PatelSUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 94305 Stanford, California, United StatesMore by Anjli Patel
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- Karen Chan*Karen Chan*[email protected]CatTheory, Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby, DenmarkMore by Karen Chan
Abstract
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.
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