Highly Matched Porous MXene Anodes and Graphene Cathodes for High-Performance Aqueous Asymmetric Supercapacitors

Aqueous asymmetric supercapacitors (ASCs) provide promising prospects for electronic systems in the future that require high energy density, power density and cycling life, due to their advantages such as low cost, safe operation and environmental friendliness. However, developing well-matched anodes and cathodes with complementary potential windows and coordinated charge storage kinetics remains a significant challenge. Here, we constructed porous MXene- and graphene-based films with nitrogenous and phosphorous terminals as anodes and cathodes, respectively, alleviating the restacking of nanosheets, generating more electrochemical active sites and improving the electrolyte penetration. The assembled aqueous ASCs based on the porous MXene and graphene films could achieve an excellent energy density of 26.8 Wh kg−1 at 425 W kg−1, high rate performance, and remarkable cycling stability with 97.3% retention after 20,000 cycles. This work demonstrates a novel concept to develop high-performance aqueous ASCs by surface engineering of two-dimensional porous electrodes with matched structural and electrochemical properties.