The lack of suitable cathodes is one of the key reasons that impede the development of aqueous zinc-ion batteries. Because of the inherently unsuitable structure and inferior physicochemical properties, the low-valent V2O3 as Zn2+ host could not be effectively discharged. Herein, we demonstrate that V2O3 (theoretical capacity up to 715 mAh g-1) can be utilized as a high-performance cathode material by an in situ anodic oxidation strategy. Through simultaneously regulating the concentration of the electrolyte and the morphology of the V2O3 sample, the ultraefficient anodic oxidation process of the V2O3 cathode was achieved within the first charging, and the mechanism was also schematically investigated. As expected, the V2O3 cathode with a hierarchical microcuboid structure achieved a nearly two-electron transfer process, enabling a high discharging capacity of 625 mAh g-1 at 0.1 A g-1 (corresponding to a high energy density of 406 Wh kg-1) and cycling stability (100% capacity retention after 10 000 cycles). This work not only sheds light on the phase transition process of low-valent V2O3 but also exploits a method toward design of advanced cathode materials.

Anodic Oxidation Strategy toward Structure-Optimized V2O3 Cathode via Electrolyte Regulation for Zn-Ion Storage