Electrofabricated Oxygen‐Terminated Zincophilic ZnCoAl‐LDH Functional Layers for Reversible Zinc Metal Anodes

Rechargeable aqueous zinc-based batteries represent a cost-effective and safe technology for grid-scale energy storage, yet are hindered by dendritic growth and parasitic reactions. Architecting artificial interface layers (AILs) exhibits a viable solution, while conventional fabrication methods often suffer from binder-induced impedance. Herein, inspired by biomedicine targeting mechanism, a binder-free, uniform ZnCoAl-layered double hydroxide interlayer enriched with zincophilic oxygen groups modified Zn anodes (LDH-O@Zn) is constructed via an integrated electrosynthesis. This well-adhered layer not only serves as a physical barrier against Zn plating-associated stress and water-induced corrosion but also dynamically regulates Zn nucleation/desolvation behaviors by terminal polar groups and unimpeded Zn²⁺ channels, thereby guiding Zn(002) preferentially homogeneous deposition. As a result, the LDH-O@Zn symmetric cell cycles stably over 2500 h at 10 mA cm⁻² and maintains an average Coulombic efficiency (CE) of 99.73% over 9000 cycles. Notably, in a full-cell configuration with a high-mass-loading NaV₃O₈·nH₂O cathode (∼19.92 mg cm⁻², N/P ratio of ∼5.45), the LDH-O@Zn delivers a remarkable capacity retention of 86.83% after 2800 cycles at 1 A g⁻¹. This work highlights the crucial role of terminal group chemistry in interfacial design, enabling scalable, durable Zn anodes for practical aqueous batteries.