Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium‐Ion Batteries

Abstract

Li₇ La₃ Zr₂ O₁₂ -based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li₂ CO₃ layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. Here, we introduce LiF to garnet Li_6.5 La₃ Zr_1.5 Ta_0.5 O₁₂ (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li₂ CO₃ on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. An all-solid-state Li/polymer/LLZT-2LiF/LiFePO₄ battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.