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

ABSTRACT 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 Zn ²⁺ 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 NaV ₃ O ₈ · n H ₂ O 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.