Decoupling the Interfacial Failure Mechanisms of Zn Anodes via Functional Zoning Strategy

Abstract The commercialization of aqueous zinc‐ion batteries is impeded by the dynamic interfacial instability of zinc anodes, stemming from the intertwined issues of dendritic growth, hydrogen evolution corrosion, and sluggish ion transport. Conventional homogeneous interfacial layers fail to decouple these conflicting requirements. Inspired by biological compartmentalization, this study proposes a molecular‐level functional zoning strategy, employing [2‐(9H‐carbazol‐9‐yl)ethyl]phosphonic acid (2PACz) to construct a self‐assembled interface layer. This design assigns distinct functions to specific molecular domains: the phosphonate group provides strong anchoring for dendrite suppression; the hydrophobic carbazole moiety blocks water and facilitates desolvation to inhibit HER; while the alkyl chain promotes ordered ion transport channels. This synergistic effect breaks the vicious cycle of interfacial degradation, reducing interfacial water density by 12% and H 2 generation by 43%. Consequently, the Zn||Zn symmetric cell achieves exceptional stability over 4000 h at 1 mA cm −2 with 17.1% DOD, and the Zn||MnO 2 full cell maintains 83.1% capacity after 3000 cycles at 3 A g −1 . This work provides a novel interfacial design and a universal molecular paradigm for advanced metal anodes.