Engineering a Ni–Al Brucite-Based Interface Layer with Regulated Zn²⁺ Flux for Highly Reversible Zn Metal Anodes

Abstract

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.

Manipulating Zn Metal Texture with Guided Zincophilic Sites via Electrochemical Stripping for Dendrite-Free Zn Anodes

“…Nowadays, the world is struggling to establish low-carbon and green ecofriendly ecosystems, which necessitates the utilization and development of clean and sustainable energy. − Cheap, reliable, and ecofriendly electrical energy storage devices will play a key role in integrating these unstable and intermissive renewable energies. , In recent years, massive postlithium new battery chemistries have been rapidly developed. − Among these battery technologies, rechargeable aqueous zinc-ion batteries (AZIBs) with the merits of low cost, operational safety, and ecofriendliness are considered one of the most promising alternatives for large-scale energy storage systems. − However, the direct contact between the aqueous electrolyte and Zn metal could induce unwanted parasitic reactions (H 2 evolution and corrosions), thus resulting in uneven plating/stripping behavior and severe byproduct accumulation. This in turn promotes the Zn dendrite’s growth, ultimately resulting in undesirable electrolyte consumption, inferior Coulombic efficiency (CE), and poor cycling durability. , Therefore, it is urgent to develop a feasible and efficient strategy to suppress multiple side reactions and Zn dendrite for the practical application of AZIBs.…”