Abstract
Abstract This work reveals the capacitive behaviors of graphene nanomaterials in typical ionic liquids of [BMI+] [BF4 −] using molecular dynamics simulations. It is found that the charging process induces a structural transition from disordered to partially ordered and then ordered multilayer structures of [BMI+][BF4 −] electrolyte, yielding a multiple layer-by-layer packing structure of BMI+ cation and BF4 − anion. Especially, a counterion-adsorption-dominated Helmholtz layer is revealed at a high charge density of 16 μC/cm2, which is primarily responsible for the superior capacitance results. Besides, the differential capacitance of [BMI+][BF4 −] exhibits a symmetric convexity-shaped curve, showing a maximal capacitance value of 4.83 μF/cm2. The as-obtain simulation results help to understand the microscopic charge storage mechanisms of graphene in ionic liquids.
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