Crumpled Nitrogen-Doped Graphene for Supercapacitors with High Gravimetric and Volumetric Performances

Graphene is considered a promising electrochemical capacitors electrode material due to its high surface area and high electrical conductivity. However, restacking interactions between graphene nanosheets significantly decrease the ion-accessible surface area and impede electronic and ionic transfer. This would, in turn, severely hinder the realization of high energy density. Herein, we report a strategy for preparation of few-layer graphene material with abundant crumples and high-level nitrogen doping. The two-dimensional graphene nanosheets (CNG) feature high ion-available surface area, excellent electronic and ion transfer properties, and high packing density, permitting the CNG electrode to exhibit excellent electrochemical performance. In ionic liquid electrolyte, the CNG electrode exhibits gravimetric and volumetric capacitances of 128 F g^-1 and 98 F cm^-3, respectively, achieving gravimetric and volumetric energy densities of 56 Wh kg^-1 and 43 Wh L^-1. The preparation strategy described here provides a new approach for developing a graphene-based supercapacitor with high gravimetric and volumetric energy densities.