Molecular Dynamics Simulations of Graphene and Graphene-Derived Ionic Liquid Supercapacitors: A Review of Methods and Applications

Abstract

Abstract Graphene and graphene-derived electrodes combined with ionic liquid electrolytes provide atomically well-defined, high-surface-area interfaces and wide electrochemical windows, making them benchmark platforms for supercapacitor research. Understanding how molecular-scale structure at this interface controls macroscopic capacitance requires molecular dynamics simulation since neither continuum theory nor experiment alone resolves the relevant length and time scales. This review treats the electrode-charging methods available─fixed and constant-charge, constant potential, electronic-structure-aware variants, and applied fields─together with force-field choice, as a toolbox of complementary tools suited to different questions, not a hierarchy of accuracy. We use this framework to organize findings on interfacial structure, electrode curvature, defects, doping, and nanoconfinement, emphasizing how these factors affect both the electric double layer and quantum capacitance. We conclude that progress toward predictive simulation will depend less on selecting a single optimal method than on integrating electrolyte polarizability, realistic electrode electronic response, structural complexity, and transferable machine-learning potentials within experimentally validated frameworks.