Bifunctional Interphase with Target‐Distributed Desolvation Sites and Directionally Depositional Ion Flux for Sustainable Zinc Anode

Abstract Aqueous zinc batteries (AZBs) feature high safety and low cost, but intricate anodic side reactions and dendrite growth severely restrict their commercialization. Herein, ethylenediaminetetraacetic acid (EDTA) grafted metal organic framework (MOF‐E) is proposed as a dually‐functional anodic interphase for sustainable Zn anode. Specifically, the target‐distributed EDTA serves as an ion‐trapped tentacle to accelerate the desolvation and ionic transport by powerful chemical coordination, while the MOFs offer suitable ionic channels to induce oriented deposition. As a result, MOF‐E interphase fundamentally suppresses side reactions and guides horizontally arranged Zn deposition with (002) preferred orientations. The Zn|MOF‐E@Cu cell exhibits a markedly improved Coulombic efficiency of 99.7 % over 2500 cycles, and the MOF‐E@Zn|KVOH (KV 12 O 30‐y ⋅ nH 2 O) cell yields a steady circulation of 5000 cycles@90.47 % at 8 A g −1 .