Janus Adsorption of Polar Ion Hubs for Simultaneous Regulation of Zinc Deposition Kinetics and Interfacial Stability in Long‐Cycle Aqueous Zinc‐Ion Batteries

Abstract Aqueous zinc‐ion batteries (AZIBs) have garnered significant attention as potential candidates for next‐generation energy storage systems, attributed to their high capacity, cost‐effectiveness, and environmentally benign nature. However, the uncontrolled proliferation of zinc dendrites and severe interfacial side reactions have emerged as substantial obstacles to their practical application. In this study, a novel “polar ionic hub regulation” strategy is introduced, which involves the covalent bonding of hydrophilic‐hydrophobic bifunctional groups to construct an asymmetric topological structure, thereby forming a nanoscale Janus interface at the molecular level. The carboxyl and amide groups synergistically anchor Zn ²⁺ ions through spatial cooperation, creating localized Zn ²⁺ ‐rich domains. Meanwhile, the benzene ring repels free water molecules via its hydrophobic effect, effectively blocking the interfacial side reactions initiated by water molecules. Consequently, the zinc anode achieves an ultralong cycling lifespan exceeding 3600 h at 1 mA cm ⁻² and 1 mAh cm ⁻² . Moreover, the zinc symmetric cell attains a cumulative plating capacity of 4.875 Ah cm ⁻² at a high areal capacity of 5 mAh cm ⁻² . Full cells paired with Na ₂ V ₆ O ₁₆ ·3H ₂ O and I ₂ cathodes exhibit significantly enhanced performance. Notably, the Zn||I ₂ system demonstrates exceptional cycling durability. This work provides a robust foundation for the practical application of high‐performance aqueous zinc‐ion batteries.