Robust Zinc Anode Enabled by Sulfonate‐Rich MOF‐Modified Separator

Abstract Aqueous zinc ion batteries (ZIBs) hold great promise for large‐scale energy storage; however, severe zinc dendritic growth and side reactions on the anode dramatically impede their commercial application. Herein, a Zr‐based MOF (UiO‐66) functionalized with a high density of sulfonic acid (─SO 3 H) groups is used to modify the glass fiber (GF) separator of ZIBs, providing a unique solution for stabilizing Zn anode. Benefiting from the strong interaction between zincophilic −SO 3 H and Zn 2+ , this sulfonate‐rich UiO‐66 modified GF (GF@UiO‐S2) separator not only guarantees the homogeneous distribution of ion flux, but also accelerates the ion migration kinetics. Hence, the GF@UiO‐S2 separator promotes uniform Zn plating/stripping on the Zn anode and facilitates the desolvation of hydrated Zn 2+ ions at the interface, which helps guide dendrite‐free Zn deposition and inhibit undesired side reactions. Accordingly, the Zn||Zn symmetric cell with this separator achieves excellent cycling stability with a long cycle life exceeding 3450 h at 3 mA cm −2 . Besides, the Zn||MnO 2 full cell paired with this separator delivers remarkable cyclability with 90% capacity retention after 1200 cycles. This design of metal–organic frameworks functionalized separators provides a new insight for constructing highly robust ZIBs.