Biomimetic Localized Gel Electrolyte for Practical Zinc Anode

Abstract Incompatible electrode/electrolyte interface often leads to dendrite growth, parasitic reactions, and corrosion, posing significant challenges to the application of Zn anodes. Herein, we introduce a biomimetic antifreeze protein localized gel electrolyte (ALGE) with multifunctional capabilities to address these issues by combining electrolyte modification with interface optimization. ALGE modifies the Zn 2+ solvation structure and the hydrogen‐bond network adjacent to the zinc anode, effectively suppressing hydrogen evolution. Additionally, ALGE promotes (002) Zn crystal plane‐dominated deposition by protein‐zinc surface interactions, enabling a long‐range dendrite‐free deposition. The absence of by‐products and inhibited corrosion further highlights the practical potential of ALGE. Symmetric cells with ALGE‐modified zinc demonstrate an impressive lifespan of 610  h under a current density of 10 mA cm −2 and a capacity of 10 mAh cm −2 . The pouch cell integrating a manganese dioxide cathode and ALGE‐modified Zn anode retains 75.8% of its capacity after 200 cycles at 1 A g −1 . This localized gel electrolyte strategy offers a practical and scalable approach to stabilizing Zn anodes for next‐generation energy storage systems.