Zincophilic–Hydrophobic Interface Design for Dendrite-Free Aqueous Zinc-Ion Batteries

Abstract Achieving Zn anode stability is critical for advancing commercialization of aqueous zinc-ion batteries. However, the instability of zinc metal anodes driven by dendritic growth, hydrogen evolution, and interfacial passivation remains a critical obstacle for advancing aqueous zinc-ion batteries. In this paper, we report a synergistic interfacial engineering strategy that integrates in situ-grown zincophilic copper nanorod arrays with a self-assembled layer of 1-dodecanethiol to regulate ion flux and suppress side reactions simultaneously. The water-poor electric double-layer microenvironment derived from this dual-function “zincophilic–hydrophobic” architecture (denoted as HS-Cu@Zn) promotes uniform Zn deposition along the (100) plane, enhances desolvation kinetics (Zn 2 + transference number increased from 0.47 to 0.75), and effectively excludes electroactive water molecules from the anode surface. As a result, the symmetric cells exhibit ultra-long cycling stability over 3500 h at 1 mA cm −2 , while Zn||Cu half-cells maintain a Coulombic efficiency of 99.65% for 900 cycles. ZnVO||HS-Cu@Zn full cell demonstrates exceptional cycling stability, achieving 2000 stable cycles at 5 A g −1 with an average Coulombic efficiency of 99.8%.