Atomic‐Level Regulation of Gibbs Free Energy for Thermodynamically Suppressing Vanadium Dissolution in V 6 O 13 Cathode Toward Stable Zinc Storage

ABSTRACT Vanadium oxides have been considered as ideal cathode materials for aqueous zinc‐ion batteries (AZIBs) due to their multivalent characteristics and open framework. Nevertheless, spontaneous vanadium dissolution and inherent low electronic conductivity of vanadium oxides result in severe capacity degradation during prolonged cycling. Herein, we propose a strategy of atomic‐level N refilling oxygen vacancy (V o ) to thermodynamically enhance the intrinsic structural strength of the V 6 O 13 cathode (V 6 O 13 ‐V o ‐N) through regulation of Gibbs free energy (ΔG = ΔH − TΔS). Theoretical calculations indicate that refilled N atoms strengthen V─O bonds by improving orbital hybridization between V 3d and O…

• NN
  National Natural Science Foundation of China

  Award: 42377487
• CP
  China Postdoctoral Science Foundation

  Award: 2025M770024