Drastically Promoting Rate Capability via Dual‐Cations Intercalation of V2O5 Enabling Rapid Zinc‐Ion Storage

Abstract Layered vanadium pentoxide (V 2 O 5 ) has drawn enormous attention as cathode material for aqueous zinc‐ion batteries (AZIBs). However, the fragile open‐framework and the sluggish Zn 2+ migration due to the strong electrostatic interaction between Zn 2+ and cathode electrode hinder the development of AZIBs. Here, an effective dual‐cations intercalation strategy is employed based on synergistic effect of Mn 2+ and Zn 2+ , which introduces guest species with robust layered construction and weak electrostatic interaction in the V 2 O 5 bulk. Consequently, the (Mn 0.13 Zn 0.03 )V 2 O 5 (abbreviated to MZVO) electrode exhibits a high reversible capacity of 463 mA h g −1 at 0.1 A g −1 , a high cycling stability (94% of capacity retention after 1000 cycles at 10 A g −1 ) and superior rate performance of 256 mAh g −1 at 20 A g −1 . The outstanding performance of MZVO cathode is attributed to the Mn 2+ ‐induced fast migration of Zn 2+ transfer and Zn 2+ ‐induced high structural stability conducted by density functional theory (DFT) calculations. The two‐phase reaction mechanism of MZVO during Zn 2+ (de)interaction is systematically expounded via operando XRD. This study will provide reference for the design of modified layered metal oxides in the future.