Sudarshan Vijay^1*, Georg Kastlunger¹, Joseph Gauthier^2,3, Anjli Patel², Karen Chan¹

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

* Corresponding authors emails: vijays@fysik.dtu.dk

DOI10.24435/materialscloud:p4-fj [version v1]

Publication date: Jun 15, 2022

How to cite this record

Sudarshan Vijay, Georg Kastlunger, Joseph Gauthier, Anjli Patel, Karen Chan, Force-based method to determine the potential dependence in electrochemical barriers, Materials Cloud Archive 2022.78 (2022), doi: 10.24435/materialscloud:p4-fj.

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.

Materials Cloud sections using this data

Files

File name	Size	Description
calculations.zip MD5md5:1def374f08ae486a7597d969be19f011	192.0 MiB	Output files of DFT calculations used to generate the figures in the manuscript. Note that a combination of DFT codes were used, and is demarcated by the folder names. NOTE: The folders contains pickle files generated by ASE v. 3.20 obtained during the vibrational calculations.

License

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Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

Electrochemical kinetics Electrochemical barriers Proton-electron transfer reactions