Different charge-storage mechanisms in disulfide vanadium and vanadium carbide monolayer

Two-dimensional (2D) transition-metal (TM) compound nanomaterials, due to their high-surface-area and large potential charge capability of TM atoms, have been widely investigated as electrochemical capacitors. However, the understanding of charge-storage mechanisms of 2D transition-metal compounds as electrode materials is still limited. In this study, using density functional theory computations, we systematically investigate the electrochemical properties of monolayer VS 2 and V 2 C. Their electronic structures show a significant electron storage capability of around 0.25 V, referenced to the standard hydrogen electrode, and indicate redox pseudocapacitance characteristics as cathodes. The different charge densities visually confirm that excess electrons tend to localize in the vanadium atoms nearby contact-adsorbed Li ions, corresponding to the redox of vanadium atoms. In contrast, only the electric double layer acts as a charge-storage mechanism in the V 2 C monolayer. However, the O saturation would induce redox pseudocapacitance in the V 2 C monolayer. Furthermore, the calculated metallic behavior and low Li ion diffusion barriers substantiate that V 2 C and VS 2 monolayers would manifest low resistance in the charging process. Our findings provide insights for the different charge-storage mechanism of VS 2 and V 2 C monolayers.