An Ionic Sieve‐Integrated Conductive Interfacial Design to Simultaneously Regulate the Zn2+ Flux and Interfacial Resistance for Advancing Zinc‐Ion Batteries

Abstract Zinc‐ion batteries possess operation safety, high energy density, production flexibility and affordability, making them attractive for scalable energy storage. While Zn anodes face significant challenges from rampant dendrite growth and electrolyte‐related side‐reactions in a complex interfacial microenvironment. The growing interfacial resistance further degrades the battery performance. An integrated anode interfacial design is reported to regulate simultaneously the Zn 2+ flux and interfacial resistance through in situ confinement growth of Zn 2+ sieve, that is, 2D CuBDC metal–organic framework in mesoporous carbonaceous host. CuBDC with sub‐nanometer channels is selected for efficient dehydration and directional Zn 2+ flux transport, and lowering the nucleation barrier by zincophilic Cu(II) and N sites. Conductive meso‐carbon reduces the interfacial resistance and blocks the interfacial side‐reactions. Resultantly, the modified Zn anodes demonstrate improved cycling stability with lower voltage polarization, supported by operando optical microscopy and ex situ analysis. This work provides a feasible strategy improving aqueous Zn anodes and new interfacial insights on designing advancing zinc batteries.