V ₂ O ₃ with Se‐Enhanced d‐p Orbital Hybridization Toward Highly Stable Aqueous Zinc Batteries under 10 A g ⁻¹

Abstract

Abstract Vanadium‐based compounds are a reliable and promising cathode material for aqueous zinc ion batteries. However, the rapid insertion/extraction of Zn 2+ at high current densities triggers irreversible structural degradation and slow ion diffusion kinetics, leading to poor cycling stability. Herein, highly conductive Se is doped into a carbon skeleton of V 2 O 3 , realizing the orbital interaction between V 3d and Se 4p orbitals. Density functional theory calculations verify that the strong d‐p orbital hybridization upshifts the d‐band center of V, optimizes the charge distribution, and reduces the Zn 2+ and H + adsorption energies. Furthermore, the robust V─Se covalent network in the Se‐V 2 O 3 @C electrode significantly enhances the electrode's redox activity and conductivity, resulting in high specific capacity and ultra‐long cycle life. Therefore, the Se‐V 2 O 3 @C‐650 electrode exhibits a high capacity of 460.87 mAh g −1 at 0.1 A g −1 . When the current density is 10 A g −1 , the capacity reaches 168.32 mAh g −1 after 10 000 cycles, with a 73.8% capacity retention after 20 000 cycles, which exceeds the reported electrodes. This work presents new insights for constructing high‐performance AZIB cathodes by establishing the mechanism of action between d‐p orbital hybridization and electrochemical performance.