Organic–Inorganic Hybrid Vanadium Oxide Cathode Material for High‐Rate and Durable Aqueous Zinc‐Ion Batteries

Abstract Vanadium oxides, known for their multi‐oxidation states and deformable V─O polyhedra, are promising cathodes for aqueous zinc‐ion batteries (AZIBs), yet suffer from limited interlayer spacing and structural instability. Here, an inorganic–organic co‐intercalated cathode (AlVO‐DMF2) is developed by partially replacing crystalline water in Al 2.65 V 6 O 13 ·2.07H 2 O with dimethylformamide (DMF). Interlayer Al 3 ⁺ serve as structural supports, preventing structural damage during the removal of crystalline water from nanobelts. They also anchor polar DMF molecules between layers via electrostatic adsorption. The strong attraction between C═O groups and Al 3 ⁺ reduces Zn 2 ⁺ affinity to DMF, facilitating reversible Zn 2 ⁺ (de)intercalation and improving structural stability. The Zn//AlVO‐DMF2 battery delivers a high average discharge capacity of 430.56 mAh·g −1 at 0.1 A·g −1 and recovers to 418.84 mAh·g −1 when the current returns to 0.05 A·g −1 after high‐rate cycling, demonstrating excellent rate capability. This study provides a promising strategy for designing advanced inorganic–organic co‐intercalated vanadium‐based cathodes for AZIBs.