Hierarchical Nanosheets/Walls Structured Carbon‐Coated Porous Vanadium Nitride Anodes Enable Wide‐Voltage‐Window Aqueous Asymmetric Supercapacitors with High Energy Density

: The energy density of aqueous asymmetric supercapacitors (ASCs) is usually limited by low potential windows and capacitances of both anode and cathode. Herein, a facile strategy to fabricate hierarchical carbon-coated porous vanadium nitride nanosheet arrays on vertically aligned carbon walls (CC/CW/p-VN@C) as anode for aqueous ASCs is reported. The potential window of CC/CW/p-VN@C electrode can be stably extended to -1.3 to 0 V (vs Ag/AgCl) with greatly improved specific capacitance (604.8 F g-1 at 1 A g-1), excellent rate capability (368 F g-1 at 60 A g-1), and remarkable electrochemical stability. To construct ASCs, a Birnessite Na0.5MnO2 nanosheet arrays (CC/CW/Na0.5MnO2) cathode is similarly built. Benefiting from the matchable potential windows and high specific capacitances of the rationally designed anode and cathode, aqueous CC/CW/p-VN@C||CC/CW/Na0.5MnO2 ASCs with a wide voltage window of 2.6 V are fabricated. Moreover, the ASCs showcase an ultrahigh energy density up to 96.7 W h kg-1 at a high power density of 1294 W kg-1, and excellent cycling stability (92.5% retention after 10 000 cycles), outperforming most of previously reported ASCs and even comparable to that of organic electrolyte supercapacitors (SCs). This efficient strategy for fabricating 2.6 V aqueous ASCs suggests a promising research system for high energy density SCs.