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  4. MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes
 
research article

MetalWalls: Simulating electrochemical interfaces between polarizable electrolytes and metallic electrodes

Coretti, Alessandro  
•
Bacon, Camille
•
Berthin, Roxanne
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November 14, 2022
Journal Of Chemical Physics

Electrochemistry is central to many applications, ranging from biology to energy science. Studies now involve a wide range of techniques, both experimental and theoretical. Modeling and simulations methods, such as density functional theory or molecular dynamics, provide key information on the structural and dynamic properties of the systems. Of particular importance are polarization effects of the electrode/electrolyte interface, which are difficult to simulate accurately. Here, we show how these electrostatic interactions are taken into account in the framework of the Ewald summation method. We discuss, in particular, the formal setup for calculations that enforce periodic boundary conditions in two directions, a geometry that more closely reflects the characteristics of typical electrolyte/electrode systems and presents some differences with respect to the more common case of periodic boundary conditions in three dimensions. These formal developments are implemented and tested in MetalWalls, a molecular dynamics software that captures the polarization of the electrolyte and allows the simulation of electrodes maintained at a constant potential. We also discuss the technical aspects involved in the calculation of two sets of coupled degrees of freedom, namely the induced dipoles and the electrode charges. We validate the implementation, first on simple systems, then on the well-known interface between graphite electrodes and a room-temperature ionic liquid. We finally illustrate the capabilities of MetalWalls by studying the adsorption of a complex functionalized electrolyte on a graphite electrode.

  • Details
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Type
research article
DOI
10.1063/5.0101777
Web of Science ID

WOS:000882459400016

Author(s)
Coretti, Alessandro  
Bacon, Camille
Berthin, Roxanne
Serva, Alessandra
Scalfi, Laura
Chubak, Iurii
Goloviznina, Kateryna
Haefele, Matthieu
Marin-Lafleche, Abel
Rotenberg, Benjamin
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Date Issued

2022-11-14

Published in
Journal Of Chemical Physics
Volume

157

Issue

18

Article Number

184801

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

temperature ionic liquids

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molecular-dynamics

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ewald summation

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force-field

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energy

•

model

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density

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charges

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surface

•

origin

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

Available on Infoscience
December 5, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/193047
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