Unlocking Ultra‐Fast Kinetics in Vanadium Oxides via the Synergistic Intercalation of Mo ⁶⁺ and PANI for Superior Zinc‐Ion Storage

ABSTRACT V‐based materials, with the high specific capacity and multi‐electron redox reactions, are considered as preferred cathodes for low‐cost and high‐safety aqueous zinc‐ion batteries. Nevertheless, poor electronic conductivity, sluggish kinetics, vanadium dissolution, and unstable structure pose severe challenges for the further practical applications. To address these issues, in this study, transition metal ions Mo 6+ and polyaniline were incorporated into V 2 O 5 derived from vanadium acetylacetonate via a one‐step hydrothermal method (MPVO). The results reveal that MPVO exhibits a unique three‐dimensional (3D) sea urchin‐like morphology with a satisfactory specific surface area and high concentration of oxygen vacancies. These characteristics offer more reaction sites for Zn 2+ and adjust the electronic conductivity. Moreover, kinetic analysis and density‐functional‐theory calculations indicate that MPVO performs metallic behavior, with the lowest Zn 2+ diffusion barrier and outstanding pseudocapacitive storage capacity. Hence, the MPVO cathode delivers a reversible capacity of approximately 457.5 mAh g −1 at 0.1 A g −1 . Moreover, it demonstrates remarkable high‐rate capacity and robust long‐cycle performance. This study realizes a triple‐strategy approach of enlarging the interlayer spacing, evolving from a zero‐dimensional (0D) to 3D sea urchin‐like morphology, and introducing abundant defects. These synergistic strategies significantly enhance the rapid kinetics and high stability of the MPVO cathode and provide new insights for designing V‐based cathodes.