Topological Amorphization of VO ₂ via Chemical Locking for Durable Aqueous Zinc‐Ion Storage

Abstract

ABSTRACT Although vanadium‐based oxides are promising cathodes for aqueous zinc‐ion batteries (AZIBs), their rigid crystalline lattices suffer from sluggish ion diffusion and rapid capacity decay caused by vanadium dissolution. Here, we report an organic‐driven topological amorphization strategy to construct a resilient and kinetically accelerated cathode. Using levamisole hydrochloride (LMS) as a dual‐functional modulator, strong Lewis's acid‐base interactions (V─N/V─S coordination) generate localized tensile stress that progressively disrupts the long‐range periodic lattice. This targeted lattice cleavage transforms crystalline VO 2 into a short‐range ordered amorphous sponge (denoted as L‐VO 2 ‐0.1), while preserving nanoclustered motifs interconnected through flexible organic “hinges”. The resulting topological architecture simultaneously reconciles the stability‐kinetics trade‐off, where the isotropic 3D open framework enables fast, sterically unimpeded Zn 2+ transport with capacitor‐like kinetics, while the dynamic organic hinges efficiently accommodate volume strain and thermodynamically suppress vanadium dissolution. Consequently, the L‐VO 2 ‐0.1 cathode delivers 481.6 mAh g −1 at 0.5 A g −1 and sustains 12 000 cycles at an extreme rate of 20 A g −1 with 83.5% capacity retention. Furthermore, a dual‐cathode pouch cell achieves a commercial‐grade absolute capacity of 1.15 Ah and a high areal capacity of 7.9 mAh cm −2 under a stringent mass loading (>20 mg cm −2 ), enabling feasible routes toward scalable, durable energy storage devices.