Zincophilic Hydrogen-Bonded Organic Frameworks with Vertical Channels Enabling Fast Ion-Transport Kinetics and Interface Stability toward Ultrastable Zn Anodes

Although aqueous zinc-ion batteries have undergone remarkable development due to their various advantages, the key zinc anode component is still hindered by severe challenges. Herein, a fast ion transport, zincophilic, and mechanically robust hydrogen-bonded organic framework (HOF) protective layer is developed on Zn metals, achieving ultrastable zinc anodes (HOF@Zn). This HOF layer exhibits oriented channels for fast Zn ion transport toward the anode interface, eliminating the concentration gradient of Zn ions. Zincophilic sites of HOFs inhibit the solvation of zinc ions, promoting their reaction kinetics and suppressing side reactions of the Zn anode. Moreover, the HOF layer reveals high mechanical stability to maintain continuous protection. Consequently, HOF@Zn exhibits surprising performances, including high Zn deposition/stripping reversibility and superior cycling stability. Even under demanding conditions (40 mA cm^-2/40 mAh cm^-2), HOF@Zn still shows a long cycle life (2577 h) and a cumulative cycle capacity (103 Ah cm^-2).