Authors: Peng Lei, Gang Wu, Hong Liu, Xiang Qi, Meng Wu, Dabing Li, Yang Li, Lei Gao, Ce‐Wen Nan, Li‐Zhen Fan
Published: 2025-02-26
Source: Full article
AbstractThe recently emerged chloride solid electrolytes have garnered significant attention due to their superior ionic conductivity, wide electrochemical stability window, and exceptional compatibility with high‐voltage oxide cathodes. Nevertheless, the currently cost‐effective Zr‐based chloride solid electrolytes face significant challenges, including low ionic conductivity and poor moisture stability. Herein, a versatile Zn2+‐doped Zr‐based chloride electrolyte is presented, designed to meet the aforementioned requirements. The optimized Li2.4Zr0.8Zn0.2Cl6 exhibits an improved ionic conductivity of 1.13 mS cm−1 at 30 °C. Simultaneously, the Li2.4Zr0.8Zn0.2Cl6 also demonstrates impressive moisture stability, maintaining its structural integrity after exposure to humid air. The mechanism underlying the enhanced moisture stability of Li2.4Zr0.8Zn0.2Cl6 is further elucidated by density functional theory calculations. Most notably, whether coupled with LiCoO2 or LiNi0.8Mn0.1Co0.1O2 cathodes, Li2.4Zr0.8Zn0.2Cl6‐based all‐solid‐state batteries demonstrate exceptional cycling stability and rate performance. This high ionic conduction and moisture‐resistant chloride electrolyte holds great promise for significantly advancing the commercialization of all‐solid‐state lithium batteries.