Work

A semiclassical Thomas–Fermi model to tune the metallicity of electrodes in molecular simulations

Year: 2020

Type: article

Abstract: Spurred by the increasing needs in electrochemical energy storage devices, the electrode/electrolyte interface has received a lot of interest in recent years. Molecular dynamics simulations play a prominent role in this field since they provide a microscopic picture of the mechanisms involved. The current state-of-the-art consists of treating the electrode as a perfect conductor, precluding the possibility to analyze the effect of its metallicity on the interfacial properties. Here, we show that the Thomas-Fermi model provides a very convenient framework to account for the screening of the electric field at the interface and differentiating good metals such as gold from imperfect conductors such as graphite. All the interfacial properties are modified by screening within the metal: the capacitance decreases significantly and both the structure and dynamics of the adsorbed electrolyte are affected. The proposed model opens the door for quantitative predictions of the capacitive properties of materials for energy storage.

Source: The Journal of Chemical Physics

DOI: 10.1063/5.0028232

Authors: Laura Scalfi, Thomas Dufils, Kyle G. Reeves, Benjamin Rotenberg, Mathieu Salanne

Institutions: Centre National de la Recherche Scientifique, Sorbonne Université, Réseau sur le Stockage Electrochimique de l'énergie, PHENIX laboratory, Institut Universitaire de France

Language: English

Topic: Electrostatics and Colloid Interactions

Subfield: Physical and Theoretical Chemistry

Field: Chemistry

Domain: Physical Sciences

Open Access status: bronze

Funders: European Commission, Agence Nationale de la Recherche, Grand Équipement National De Calcul Intensif, H2020 European Research Council