Zn-based electrochemical energy storage (EES) systems have received tremendous attention in recent years, but their zinc anodes are seriously plagued by the issues of zinc dendrite and side reactions (e.g., corrosion and hydrogen evolution). Herein, we report a novel strategy of employing zincophilic Cu nanowire networks to stabilize zinc anodes from multiple aspects. According to experimental results, COMSOL simulation and density functional theory calculations, the Cu nanowire networks covering on zinc anode surface not only homogenize the surface electric field and Zn2+ concentration field, but also inhibit side reactions through their hydrophobic feature. Meanwhile, facets and edge sites of the Cu nanowires, especially the latter ones, are revealed to be highly zincophilic to induce uniform zinc nucleation/deposition. Consequently, the Cu nanowire networks-protected zinc anodes exhibit an ultralong cycle life of over 2800 h and also can continuously operate for hundreds of hours even at very large charge/discharge currents and areal capacities (e.g., 10 mA cm−2 and 5 mAh cm−2), remarkably superior to bare zinc anodes and most of currently reported zinc anodes, thereby enabling Zn-based EES devices to possess high capacity, 16,000-cycle lifespan and rapid charge/discharge ability. This work provides new thoughts to realize long-life and high-rate zinc anodes.

Ultrathin separators are indispensable to high‐energy‐density zinc‐ion batteries (ZIBs), but their easy failure caused by zinc dendrites poses a great challenge. Herein, 23 µm‐thick functional ultrathin separators (FUSs), realizing superb electrochemical stability of zinc anodes and outstanding long‐term durability of ultrathin separators, are reported. In the FUSs, an ultrathin but mechanically strong nanoporous membrane substrate benefits fast and flux‐homogenized Zn2+ transport, while a metal–organic framework (MOF)‐derived C/Cu nanocomposite decoration layer provides rich low‐barrier zinc nucleation sites, thereby synergistically stabilizing zinc anodes to inhibit zinc dendrites and dendrite‐caused separator failure. Investigation of the zinc affinity of the MOF‐derived C/Cu nanocomposites unravels the high zincophilicity of heteroatom‐containing C/Cu interfaces. Zinc anodes coupled with the FUSs present superior electrochemical stability, whose operation lifetime exceeds 2000 h at 1 mA cm−2 and 600 h at 10 mA cm−2, 40–50 times longer than that of the zinc anodes using glass‐fiber separators. The reliability of the FUSs in ZIBs and zinc‐ion hybrid supercapacitors is also validated. This work proposes a new strategy to stabilize zinc anodes and provides theoretical guidance in developing ultrathin separators for high‐energy‐density zinc‐based energy storage.

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