A semiclassical Thomas-Fermi model to tune the metallicity of electrodes in molecular simulations
| Autor: | Kyle G. Reeves, Laura Scalfi, Thomas Dufils, Benjamin Rotenberg, Mathieu Salanne |
|---|---|
| Přispěvatelé: | PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX (PHENIX), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA), ANR-17-CE09-0046,NEPTUNE,Transport hors equilibre de fluides aux échelles nanométriques(2017), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM) |
| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
[PHYS]Physics [physics]
Condensed Matter - Materials Science Materials science Field (physics) Condensed matter physics Capacitive sensing General Physics and Astronomy Materials Science (cond-mat.mtrl-sci) FOS: Physical sciences 02 engineering and technology Electrolyte 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Capacitance 0104 chemical sciences Electrode Physical and Theoretical Chemistry Perfect conductor 0210 nano-technology Thomas–Fermi model Electrical conductor |
| Zdroj: | Journal of Chemical Physics Journal of Chemical Physics, 2020, 153 (17), pp.174704. ⟨10.1063/5.0028232⟩ The Journal of Chemical Physics Journal of Chemical Physics, American Institute of Physics, 2020, 153 (17), pp.174704. ⟨10.1063/5.0028232⟩ |
| ISSN: | 0021-9606 1089-7690 |
| Popis: | 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 proeminent role in this field since they provide a microscopic picture of the mechanisms involved. The current state-of-the-art consists in 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 differenciating 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. 10 pages, 10 figures (contains the SI) |
| Databáze: | OpenAIRE |
| Externí odkaz: |
|