High Volumetric Energy Density Asymmetric Supercapacitors Based on Well‐Balanced Graphene and Graphene‐MnO₂ Electrodes with Densely Stacked Architectures

The well‐matched electrochemical parameters of positive and negative electrodes, such as specific capacitance, rate performance, and cycling stability, are important for obtaining high‐performance asymmetric supercapacitors. Herein, a facile and cost‐effective strategy is demonstrated for the fabrication of 3D densely stacked graphene (DSG) and graphene‐MnO 2 (G‐MnO 2 ) architectures as the electrode materials for asymmetric supercapacitors (ASCs) by using MnO 2 ‐intercalated graphite oxide (GO‐MnO 2 ) as the precursor. DSG has a stacked graphene structure with continuous ion transport network in‐between the sheets, resulting in a high volumetric capacitance of 366 F cm –3 , almost 2.5 times than that of reduced graphene oxide, as well as long cycle life (93% capacitance retention after 10 000 cycles). More importantly, almost similar electrochemical properties, such as specific capacitance, rate performance, and cycling stability, are obtained for DSG as the negative electrode and G‐MnO 2 as the positive electrode. As a result, the assembled ASC delivers both ultrahigh gravimetric and volumetric energy densities of 62.4 Wh kg –1 and 54.4 Wh L –1 (based on total volume of two electrodes) in 1 m Na 2 SO 4 aqueous electrolyte, respectively, much higher than most of previously reported ASCs in aqueous electrolytes.