Carbon Superstructure‐Supported Half‐Metallic V₂O₃ Nanospheres for High‐Efficiency Photorechargeable Zinc Ion Batteries

Photorechargeable zinc ion batteries (PZIBs), which can directly harvest and store solar energy, are promising technologies for the development of a renewable energy society. However, the incompatibility requirement between narrow band gap and wide coverage has raised severe challenges for high‐efficiency dual‐functional photocathodes. Herein, half‐metallic vanadium (III) oxide (V 2 O 3 ) was first reported as a dual‐functional photocathode for PZIBs. Theoretical and experimental results revealed its unique photoelectrical and zinc ion storage properties for capturing and storing solar energy. To this end, a synergistic protective etching strategy was developed to construct carbon superstructure‐supported V 2 O 3 nanospheres (V 2 O 3 @CSs). The half‐metallic characteristics of V 2 O 3 , combined with the three‐dimensional superstructure assembled by ultrathin carbon nanosheets, established rapid charge transfer networks and robust framework for efficient and stable solar‐energy storage. Consequently, the V 2 O 3 @CSs photocathode delivered record zinc ion storage properties, including a photo‐assisted discharge capacities of 463 mA ⋅ h ⋅ g −1 at 2.0 A ⋅ g −1 and long‐term cycling stability over 3000 cycles. Notably, the PZIBs assembled using V 2 O 3 @CSs photocathodes could be photorecharged without an external circuit, exhibiting a high photo conversion efficiency (0.354 %) and photorecharge voltage (1.0 V). This study offered a promising direction for the direct capture and storage of solar energy.