Bottom-up dense zinc electrodeposition mediated by hydrophobic redox-active coating for ultralong-life aqueous Zn-metal batteries
Liansheng Li, Yakui Duan, Yinlong Cheng, Pengyu Meng, Wenjie Jiang, Qinghua Liang
Abstract
Uncontrolled dendrite growth and severe interfacial side reactions continue to hinder the practical deployment of Zn metal anodes in aqueous batteries. Herein, we design a multifunctional hydrophobic interfacial coating composed of 2,4,5-trifluorophenylacetate and polyvinylidene fluoride to significantly improve the cycling stability and reversibility of Zn anodes. This redox-active coating promotes uniform Zn deposition by homogenizing the electron and Zn 2+ ions distribution through preferential and reversible redox reactions. Simultaneously, the coating releases Y 3+ ions via ion exchange, which electrostatically shield surface protrusions, guiding Zn 2+ transport for bottom-up deposition beneath the insulating film. The hydrophobic nature of the coating also accelerates Zn 2+ desolvation and mechanically suppresses dendrite growth, collectively enabling dense and stable Zn plating. As a result, the optimized PY150@Zn anode achieves over 4100 h of stable cycling at 1.0 mA cm −2 with a specific capacity of 1.0 mAh cm −2 . This coating also improves full-cell performance in Zn‖V 2 O 5 batteries by mitigating anode corrosion. The proposed “three-in-one” strategy—regulating ion flux, enhancing desolvation, and suppressing dendrite formation—offers a generalizable pathway toward high-performance aqueous metal batteries.