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Title: Unified polarizable electrode models for open and closed circuits: Revisiting the effects of electrode polarization and different circuit conditions on electrode–electrolyte interfaces
Authors: Takahashi, Ken
Nakano, Hiroshi
Sato, Hirofumi
Author's alias: 高橋, 健
中農, 浩史
佐藤, 啓文
Issue Date: 7-Jul-2022
Publisher: AIP Publishing
Journal title: The Journal of Chemical Physics
Volume: 157
Issue: 1
Thesis number: 014111
Abstract: A precise understanding of the interfacial structure and dynamics is essential for the optimal design of various electrochemical devices. Herein, we propose a method for classical molecular dynamics simulations to deal with electrochemical interfaces with polarizable electrodes under the open circuit condition. Less attention has been given to electrochemical circuit conditions in computation despite being often essential for a proper assessment, especially comparison between different models. The present method is based on the chemical potential equalization principle, as is a method developed previously to deal with systems under the closed circuit condition. These two methods can be interconverted through the Legendre transformation so that the difference in the circuit conditions can be compared on the same footing. Furthermore, the electrode polarization effect can be correctly studied by comparing the present method with conventional simulations with the electrodes represented by fixed charges, since both of the methods describe systems under the open circuit condition. The method is applied to a parallel-plate capacitor composed of platinum electrodes and an aqueous electrolyte solution. The electrode polarization effects have an impact on the interfacial structure of the electrolyte solution. We found that the difference in circuit conditions significantly affects the dynamics of the electrolyte solution. The electric field at the charged electrode surface is poorly screened by the nonequilibrium solution structure in the open circuit condition, which accelerates the motion of the electrolyte solution.
Rights: © 2022 Author(s). Published under an exclusive license by AIP Publishing.
This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in ['The Journal of Chemical Physics', 157, 014111 (2022)] and may be found at https://aip.scitation.org/doi/abs/10.1063/5.0093095.
The full-text file will be made open to the public on 07 July 2023 in accordance with publisher's 'Terms and Conditions for Self-Archiving'.
URI: http://hdl.handle.net/2433/275804
DOI(Published Version): 10.1063/5.0093095
PubMed ID: 35803827
Appears in Collections:Journal Articles

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