Cation-Disordered Structure in Li₃VO₄ Anodes Achieved via Simple Spray-Drying for Unprecedented Rate Capability

Cation-disordered materials offer attractive potential for high-power energy storage by unlocking diversified ionic transport pathways, yet their practical realization remains challenging due to difficulties in stabilizing disorder. Here, we demonstrate spray-drying as a direct and scalable route to synthesize cation-disordered Li3VO4 without requiring postannealing or additional lithiation steps. By leveraging ultrafast solvent removal, this method induces flash crystallization in less than 1 s, kinetically “freezing” the metastable disordered phase. Structural analysis using synchrotron X-ray diffraction, Pair-Distribution Function analysis, and high-resolution Transmission Electron Microscopy reveals that ultrafast drying disrupts long-range cation ordering while preserving short-range periodicity, forming local cation-ordered domains within an average disordered structure. This nanoscale disorder, stabilized by antiphase domain boundaries, enhances lithium-ion diffusivity, delivering a high-power performance of 138 mAh g–1 at a 60C rate. By enabling precise control of cation disorder through drying kinetics, this study establishes spray-drying as a powerful and scalable platform for next-generation energy storage materials.