Practical Considerations for Continuum Models Applied to Surface Electrochemistry
Abstract
Abstract Modelling the electrolyte at the electrochemical interface remains a major challenge in ab initio simulations of charge transfer processes at surfaces. Recently, the development of hybrid polarizable continuum models/ ab initio models have allowed for the treatment of solvation and electrolyte charge in a computationally efficient way. However, challenges remain in its application. Recent literature has reported that large cell heights are required to reach convergence, which presents a serious computational cost. Furthermore, calculations of reaction energetics require costly iterations to tune the surface charge to the desired potential. In this work, we present a simple capacitor model of the interface that illuminates how to circumvent both of these challenges. We derive a correction to the energy for finite cell heights to obtain the large cell energies at no additional computational expense. We furthermore demonstrate that the reaction energetics determined at constant charge are easily mapped to those at constant potential, which eliminates the need to apply iterative schemes to tune the system to a constant potential. These developments together represent more than an order of magnitude reduction of the computational overhead required for the application of polarizable continuum models to surface electrochemistry.
- Authors:
-
- Stanford Univ., CA (United States)
- Technical Univ. of Denmark, Lyngby (Denmark)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1560678
- Alternate Identifier(s):
- OSTI ID: 1576648
- Grant/Contract Number:
- AC02-76SF00515; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemPhysChem
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 22; Journal ID: ISSN 1439-4235
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Gauthier, Joseph A., Dickens, Colin F., Ringe, Stefan, and Chan, Karen. Practical Considerations for Continuum Models Applied to Surface Electrochemistry. United States: N. p., 2019.
Web. doi:10.1002/cphc.201900536.
Gauthier, Joseph A., Dickens, Colin F., Ringe, Stefan, & Chan, Karen. Practical Considerations for Continuum Models Applied to Surface Electrochemistry. United States. https://doi.org/10.1002/cphc.201900536
Gauthier, Joseph A., Dickens, Colin F., Ringe, Stefan, and Chan, Karen. Wed .
"Practical Considerations for Continuum Models Applied to Surface Electrochemistry". United States. https://doi.org/10.1002/cphc.201900536. https://www.osti.gov/servlets/purl/1560678.
@article{osti_1560678,
title = {Practical Considerations for Continuum Models Applied to Surface Electrochemistry},
author = {Gauthier, Joseph A. and Dickens, Colin F. and Ringe, Stefan and Chan, Karen},
abstractNote = {Abstract Modelling the electrolyte at the electrochemical interface remains a major challenge in ab initio simulations of charge transfer processes at surfaces. Recently, the development of hybrid polarizable continuum models/ ab initio models have allowed for the treatment of solvation and electrolyte charge in a computationally efficient way. However, challenges remain in its application. Recent literature has reported that large cell heights are required to reach convergence, which presents a serious computational cost. Furthermore, calculations of reaction energetics require costly iterations to tune the surface charge to the desired potential. In this work, we present a simple capacitor model of the interface that illuminates how to circumvent both of these challenges. We derive a correction to the energy for finite cell heights to obtain the large cell energies at no additional computational expense. We furthermore demonstrate that the reaction energetics determined at constant charge are easily mapped to those at constant potential, which eliminates the need to apply iterative schemes to tune the system to a constant potential. These developments together represent more than an order of magnitude reduction of the computational overhead required for the application of polarizable continuum models to surface electrochemistry.},
doi = {10.1002/cphc.201900536},
journal = {ChemPhysChem},
number = 22,
volume = 20,
place = {United States},
year = {Wed Jul 17 00:00:00 EDT 2019},
month = {Wed Jul 17 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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