High-Entropy Oxide Interlayers Enable Coordinated Regulation of Zn ²⁺ Interfacial Kinetics for Stable Zinc Metal Anodes

The reversibility of Zn metal anodes in aqueous zinc–ion batteries is fundamentally limited by interfacial kinetic heterogeneity, where sluggish Zn2+ desolvation, uncontrolled surface migration, and nonuniform charge transfer jointly trigger dendrite growth and parasitic reactions. Here, we demonstrate a conformal high-entropy spinel oxide, (CrCoFeMnNi)3O4, as an interfacial layer to actively regulate Zn2+ interfacial kinetics rather than passively blocking deposition. Electrochemical impedance spectroscopy, Arrhenius analysis, and distribution of relaxation times reveal that the high-entropy oxide simultaneously lowers the Zn2+ desolvation energy barrier, suppresses lateral surface migration, and stabilizes charge-transfer and diffusion processes, thereby enabling uniform Zn plating and reversible stripping. Consequently, the modified Zn anodes achieve a Coulombic efficiency of 98.26% over 400 cycles, sustain stable symmetric cell operation for over 1100 h, and maintain low polarization at current densities up to 10 mA cm–2. When paired with NH4V4O10 cathodes, the full cells deliver 251.5 mAh g–1 after 1000 cycles and retain 138.1 mAh g–1 at 10 A g–1. This work establishes high-entropy oxide interlayers as an effective platform for mechanistically regulating Zn interfacial kinetics, offering a concise and scalable strategy for stabilizing Zn metal anodes.