Ternary Zinc-Aluminum-Bismuth Layered Double Hydroxide as an Artificial Solid Interface Protective Layer for Aqueous Zinc-Ion Battery Anodes

Aqueous zinc-ion batteries have shown great potential in large-scale energy storage due to their high safety, low cost, and environmental friendliness. However, zinc metal anodes are plagued by uncontrollable dendrite growth and side reactions, which severely limit their cycle life and practical application. To tackle these challenges, this paper proposes an innovative interface engineering strategy: a dense and robust ternary zinc-aluminum-bismuth layered double hydroxide (ZAB-LDH) protective layer is in situ grown on the zinc foil surface through a hydrothermal method, denoted as ZAB-LDH@Zn. In comparison with the zinc-aluminum binary LDH-modified zinc anode (ZA-LDH@Zn) and the bare Zn anode, the incorporation of elemental bismuth in the ternary LDH interface layer can more effectively homogenize the zinc-ion flow, inhibit hydrogen evolution and corrosion, and enhance the electrode interface stability. The assembled ZAB-LDH@Zn‖ZAB-LDH@Zn symmetrical battery exhibits a cycle life of 1800 h at 8 mA cm−2 and 1 mAh cm−2 and maintains stable operation for 225 h at 8 mA cm−2 and 8 mAh cm−2. The ZAB-LDH@Zn‖Cu half-cell attains an average coulombic efficiency of 98.5% over 635 h, demonstrating excellent zinc deposition/dissolution reversibility. The ZAB-LDH@Zn‖MnO2 full cell also exhibits excellent rate performance and long-term cycle stability. This research not only confirms the great potential of zinc-aluminum-bismuth ternary layered double hydroxide as a high-performance protective layer for zinc metal anodes but also offers novel insights for addressing the interface challenges in metal battery anodes via the design of multielement layered double hydroxides.