Engineering a Ni-Al Brucite-Based Interface Layer with Regulated Zn 2+ Flux for Highly Reversible Zn Metal Anodes.

Practical aqueous Zn-ion batteries are appealing for grid-scale energy storage with intrinsic safety and cost-effectiveness, yet their cycling stability and reversibility are limited by unwanted dendrite growth and water-induced erosions on Zn. Herein, a hydrophilic and Zn ²⁺ -conductive Ni-Al layered double hydroxide (NiAl-LDH) interphase layer is constructed on the surface of Zn, in which NiAl-LDH enables a more uniformly distributed Zn ²⁺ concentration and interfacial electric field owing to its large internal Zn ²⁺ channels and favorable charge redistribution effect. Consequently, the NiAl-LDH-integrated Zn anode achieves low voltage hysteresis and high reversibility of Zn plating/stripping with uniform underneath deposition behaviors. Remarkably, the resultant NiAl-2 LDH@Zn delivers superior cycling durability over 2800 h (∼4 months, 0.5 mA cm ^-2 ), realizes high reversibility with 99.4% average Coulombic efficiency over 1400 cycles, and confers stable operation of full Zn cells with high V ₂ O ₅ mass loadings. This work offers a facile and instructive interface design approach for achieving highly stable Zn metal anodes.