Interface Coordination Stabilizing Reversible Redox of Zinc for High‐Performance Zinc‐Iodine Batteries

Abstract Aqueous Zn batteries (AZBs) have attracted extensive attention due to good safety, cost‐effectiveness, and environmental benignity. However, the sluggish kinetics of divalent zinc ion and the growth of Zn dendrites severely deteriorate the cycling stability and specific capacity. The authors demonstrate modulation of the interfacial redox process of zinc via the dynamic coordination chemistry of phytic acid with zinc ions. The experimental results and theoretical calculation reveal that the in‐situ formation of such inorganic–organic films as a dynamic solid‐electrolyte interlayer is efficient to buffer the zinc ion transfer via the energy favorable coordinated hopping mechanism for the reversible zinc redox reactions. Especially, along the interfacial coating layer with porous channel structure is able to regulate the solvation structure of zinc ions along the dynamic coordination of the phytic acid skeleton, efficiently inhibiting the surface corrosion of zinc and dendrite growth. Therefore, the resultant Zn anode achieves low voltage hysteresis and long cycle life at rigorous charge and discharge circulation for fabricating highly robust rechargeable batteries. Such an advanced strategy for modulating ion transport demonstrates a highly promising approach to addressing the basic challenges for zinc‐based rechargeable batteries, which can potentially be extended to other aqueous batteries.