首页|Constant charge method or constant potential method:Which is better for molecular modeling of electrical double layers?

Constant charge method or constant potential method:Which is better for molecular modeling of electrical double layers?

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In molecular modeling of electrical double layers(EDLs),the constant charge method(CCM)is prized for its computational efficiency but cannot maintain electrode equipotentiality like the more resource-intensive constant potential method(CPM),potentially leading to inaccuracies.In certain scenarios,CCM can yield results identical to CPM.However,there are no clear guidelines to determine when CCM is sufficient and when CPM is required.Here,we conduct a series of molecular simulations across various electrodes and electrolytes to present a comprehensive comparison between CCM and CPM under different charging modes.Results reveal that CCM approximates CPM effectively in capturing equilibrium EDL and current-driven dynamics in open electrode systems featuring ionic liquids or regular concentra-tion aqueous electrolytes,while CPM is indispensable in scenarios involving organic and highly concen-trated aqueous electrolytes,nanoconfinement effects,and voltage-driven dynamics.This work helps to select appropriate methods for modeling EDL systems,prioritizing accuracy while considering computa-tional efficiency.

Electrochemical interfaceMolecular dynamicsElectrode polarization modelingNanoconfinement effect

Liang Zeng、Xi Tan、Xiangyu Ji、Shiqi Li、Jinkai Zhang、Jiaxing Peng、Sheng Bi、Guang Feng

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State Key Laboratory of Coal Combustion,School of Energy and Power Engineering,Huazhong University of Science and Technology(HUST),Wuhan 430074,Hubei,China

Sorbonne Université,CNRS,Physico-chimie des Électrolytes et Nanosystèmes Interfaciaux,PHENIX,F-75005 Paris,France

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaProgram for HUST Academic Frontier Youth Team

T232501252161135104

2024

10.1016/j.jechem.2024.02.043

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.94(7)