Capacitance of edge-free three-dimensional graphene: New perspectives on the design of carbon structures for supercapacitor applications

The current target for expanding the application scope of supercapacitors is to increase their energy density (E) beyond 20 Wh kg−1. In this regard, edge-free carbon materials show considerable potential because of their high working voltage (U) in organic electrolytes; however, their capacitance (C) remains limited. In this study, we synthesized edge-free three-dimensional (3D) graphene materials with different numbers of graphene stacking layers (nstack). These carbon materials have similar pore morphologies and an edge-free structure because a template method and annealing at 1800 °C were applied, respectively. These features allowed C to remain unaffected by the pore size effect, wettability, parasitic side reactions, and pseudocapacitance. Our results suggested that increasing nstack slightly enhances the areal C; however, such an increase cannot compensate for the decrease in C attributed to the decrease in the specific surface area. We also confirmed that the C of 3D graphene materials has a quantum origin, which results in a “butterfly shaped” cyclic voltammetry curve; we also successfully quantified the quantum capacitance (CQ) for the complete understanding of the origin of C. Based on this knowledge, we estimated that this 3D graphene material can yield a high E of 43 Wh kg−1 once CQ is optimized.