Accounting for the Quantum Capacitance of Graphite in Constant Potential Molecular Dynamics Simulations

• DOI: 10.1002/adma.202405230
• Publication Date: 2024-08-03T07:45:17Z
• Authors: Kateryna Goloviznina; Johann Fleischhaker; Tobias Binninger; Benjamin Rotenberg; Heigo Ers; Vladislav Ivanistsev; Robert Meissner; Alessandra Serva; Mathieu Salanne
• Keywords: Quantum capacitance

Molecular dynamics (MD) simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite numerous advances in simulation of electrodes, they fail accurately represent electronic structure materials such as graphite. In this work, simple parameterization method that allows tune metallicity electrode based quantum chemistry calculation density states (DOS) is introduced. As first illustration, interface between graphite electrodes two different liquid electrolytes, aqueous solution NaCl pure ionic liquid, applied potentials studied. It shown reproduce qualitatively experimentally-measured capacitance; particular, yield minimum capacitance point zero charge (PZC), which due (QC) contribution. An analysis adsorbed liquids understand why displays lower despite its large concentration. addition relevance for important class carbonaceous can be any (e.g. 2D materials, conducting polymers, etc), thus enabling molecular studies complex devices future.