An Artificial Interphase with Ion‐Selective Pathways Enhancing Interfacial Kinetics for Highly Reversible Zinc Anodes

ABSTRACT Aqueous zinc metal batteries (AZMBs), recognized as a prospective technology for next‐generation energy storage, face challenges including harmful parasitic reactions, and dendrite growth. Herein, a novel artificial interphase, comprising carboxylated cellulose (CNF) and β‐cyclodextrin (β‐CD), was constructed on the Zn anode (CCM@Zn). Due to the steric hindrance effect of supramolecular β‐CD, the structure of pristine CNF is rebuilt, and the CCM interphase possesses more amorphous regions, effectively accelerating Zn ²⁺ migration, and enhancing Zn ²⁺ transport kinetics. Simultaneously, the β‐CD, as an anion receptor, anchors SO ₄ ²⁻ anions to restrict their mobility, and achieve ion‐selective transport. Moreover, numerous hydroxyl groups are exposed in the CCM interphase, efficiently trapping active water and suppressing anode corrosion. Notably, CCM interphase presents outstanding mechanical ability to accommodate anode volume changes during plating. Benefiting from these advantages, CCM@Zn achieves excellent lifespans of over 2200 h at 1 mA cm ⁻² /1 mAh cm ⁻² and retains 99.88% Coulombic efficiency over 1300 cycles at 5 mA cm ⁻² in Zn||Cu cells. The CCM@Zn||MnO ₂ full cells deliver 78.32% capacity retention after 2200 cycles, with the initial capacity of 115.2 mAh g ⁻¹ at 4 A g ⁻¹ . These results provide a new interfacial engineering strategy for developing highly reversible AZMBs.