Engineering Low‐Coordination Atoms into Zn2Ti3O8 for Stable Zn Metal Anodes

Abstract The full potential realization of aqueous Zn metal‐based batteries (AZMBs) is contingent upon Zn anode stability. Modifying zincophilic protective layers can significantly enhance the Zn anode performance by reducing dendrite formation and minimizing side reactions. Principles for screening and designing zinophilic interfaces remain undeveloped. Here, a low‐coordination atom (LCA) design to guide the protective layer construction for Zn anodes is proposed. Oxygen vacancies are introduced in Zn 2 Ti 3 O 8 (ZTO x ) to reduce the coordination numbers of Ti and Zn atoms, thereby altering the electronic densities near the Fermi level of ZTO x to facilitate favorable interactions with Zn 2+ ions. Experimental and theoretical findings demonstrate enhanced zincophilic sites and charge‐reinforced interfaces resulting from the LCA design. Leveraging Zn anode interfacial chemistry regulation, the Zn@ZTO x electrodes present exceptionally planar Zn deposition. The weakened adsorption between H and ZTO x effectively prohibits side reactions. This results in Zn@ZTO x ‐based symmetric cells achieving outstanding cycling performance, with a cumulative plating capacity of 8 Ah cm −2 at 10 mA cm −2 . The full cell, coupled with an NH 4 V 4 O 10 cathode, sustains a high specific capacity of 221.6 mAh g −1 after 3000 cycles. The LCA strategy thus expands the range of potential protective materials for Zn anodes and underscores their practicability for AZMB applications.