Ultrafast Plasma‐Assisted Synthesis of Bio‐Inspired Bi‐Functional Interlayer on Zinc Anode with Enhanced Lewis‐Base Sites for Long‐Life Zinc‐Iodine Batteries

Abstract Aqueous zinc‐iodine batteries hold significant potential for large‐scale energy storage, but are hindered by the challenges such as polyiodide‐induced corrosion, dendrite formation, and other side reactions at the zinc anode. Inspired by the ion‐selective functionality of plant roots, a ZnSn(OH)₆ (ZSH) interlayer with rich Lewis‐base sites is designed to protect Zn anode. Density function theory (DFT) calculations predict that the ZSH layer can act as bi‐functional layer which selectively adsorbs Zn²⁺ while repels I₃⁻. Guided by calculations, the ZSH interlayer is rapidly constructed on Zn anode within 2 min using a dielectric barrier discharge (DBD) plasma‐assisted synthesis method. As expected, the DBD‐ZSH@Zn anode demonstrates over 5000 h of stable cycling at 5 mA cm⁻² and enables Zn–I₂ batteries to operate for 138 000 cycles at 10 A g⁻¹. It is evidenced that the DBD‐ZSH interlayer with more surface‐exposed Lewis‐base sites can facilitate Zn²⁺ desolvation and accelerate Zn²⁺ transport, leading to dendrite‐free Zn deposition. It can also protect the Zn anode from the corrosion of SO₄²⁻/I₃⁻ anions, thereby effectively mitigating side reactions. The proposed design strategy of bi‐functional protective interlayer for zinc anode and the developed DBD plasma‐assisted synthesis method will be helpful for the development of high‐performance aqueous zinc‐based batteries.