Force-Based Method to Determine the Potential Dependence in Electrochemical Barriers

Sudarshan Vijay*, Georg Kastlunger, Joseph A. Gauthier, Anjli Patel, Karen Chan*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review


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.

Original languageEnglish
JournalJournal of Physical Chemistry Letters
Issue number25
Pages (from-to)5719-5725
Publication statusPublished - 2022


Dive into the research topics of 'Force-Based Method to Determine the Potential Dependence in Electrochemical Barriers'. Together they form a unique fingerprint.

Cite this