Biomimetic Multilayer Solid‐Electrolyte Interphase Customization for Long‐Lifespan Practical Aqueous Zinc‐Metal Batteries

ABSTRACT

Aqueous zinc metal batteries are hindered by the prominent interfacial issues of the Zn anode, such as dendrite growth and intricate side reactions. The in situ construction of a stable solid‐electrolyte interphase (SEI) to address these issues remains a critical challenge, especially under high current density and harsh temperature conditions. Herein, inspired by the absorption of nutrients through plant epidermis, a gradient biomimetic multilayer self‐assembled SEI is constructed. This multilayer biomimetic SEI integrates an outer hydrophobic layer that repels water molecules to create a water‐poor interface, suppressing hydrogen evolution and facilitating Zn ²⁺ desolvation. The middle‐crosslinked layer stabilizes the SEI structure and captures SO ₄ ²⁻ to mitigate side reactions, enabling dynamic interfacial regulation. Meanwhile, the innermost adsorption layer regulates Zn ²⁺ flux, promoting uniform planar deposition along the (002) crystal plane. Benefiting from the existence of biomimetic gradient SEI, the Zn||Zn cell delivers a cycling life of over 2250 h at 20 mA cm ⁻² , and at ultrahigh current densities (50 and 100 mA cm ⁻² ), it delivers 12 250 and 1200 cycles, respectively. Furthermore, the pouch cells coupled with I ₂ deliver 1.6 Ah. This bioinspired, customizable multilayer SEI achieves Ah‐scale performance and wide‐temperature adaptability, providing valuable insights into the advancement of practical aqueous batteries.