Topological Amorphization of VO2 via Chemical Locking for Durable Aqueous Zinc-Ion Storage.

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 VO2 into a short-range ordered amorphous sponge (denoted as L-VO2-0.1), 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 Zn2+ transport with capacitor-like kinetics, while the dynamic organic hinges efficiently accommodate volume strain and thermodynamically suppress vanadium dissolution. Consequently, the L-VO2-0.1 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.