Zeolite-Based Solid-State Electrolyte for Highly Stable Zinc Metal Batteries

Abstract

Solid-state electrolytes are demonstrated great inhibition effect on cathodic dissolution and anodic side reactions in zinc-ion batteries. In this work, a novel zeolite-based solid electrolyte (Zeolite-Zn) enriched with zinc ions, high ionic conductivity (2.54 mS cm⁻¹) and high Zn²⁺ transference number (0.866) is prepared through ion-exchange strategy. Owing to the anhydrous characteristic, Zeolite-Zn electrolyte effectively extends the electrochemical window to 2.5 V and inhibits hydrogen evolution reaction. As for Zn||Zeolite-Zn||NH₄V₄O₁₀ batteries, high-capacity retention rate of 84.9% can be achieved after 1010 cycles at 0.5 A g⁻¹. Even at high temperature of 60 °C, the NH₄V₄O₁₀ cathode is able to maintain high reversible capacity of 239.2 mAh g⁻¹ after 110 cycles, which can be attributed to the superior structural stability, weak interfacial side reaction, low zinc migration barrier, and inhibited vanadium dissolution of Zeolite-Zn electrolyte. In addition, the as-fabricated Zn||Zeolite-Zn||AC@I₂ batteries have also demonstrated brilliant performances, suggesting its promising potential in practical application of zinc-based secondary batteries. This study provides mechanistic insights and structural inspiration for the original design of inorganic solid electrolytes.