Architecting a Hydrated Ca_0.24V₂O₅ Cathode with a Facile Desolvation Interface for Superior-Performance Aqueous Zinc Ion Batteries

Vanadium-based materials are promising cathode candidates for low-cost and high-safety aqueous zinc–ion batteries (AZIBs). However, they suffer from inferior rate capability and undesirable capacity fading due to their intrinsic poor conductivity and structural instability. Herein, we synthesize hydrated Ca0.24V2O5·0.75H2O (CaVOH) nanoribbons with in situ incorporations of the carbon nanotubes via a one-step hydrothermal method, achieving an integrated architecture hybrid cathode (C/CaVOH) design. Benefitting from the robust structure and low desolvation interface, the prefabricated C/CaVOH cathodes deliver a high capacity of 384.2 mA h g–1 at 0.5 A g–1 with only 5.6% capacity decay over 300 cycles, enable an ultralong cycling life of 10,000 cycles at 20.0 A g–1 with 80.2% capacity retention, and exhibit an impressive rate capability (165 mA h g–1 at 40.0 A g–1) with a high mass loading of ∼4 mg cm–2. Moreover, through the theoretical calculations and a series of ex situ characterizations, we demonstrate the Zn2+/H+ co-intercalation storage mechanism, the key role of the gallery water, and the function of the induced C–O groups in promoting kinetics of the C/CaVOH electrode. This work highlights the strategy of in situ implanted high conductivity materials to engineer vanadium-based or other cathodes for high-performance AZIBs.