A family of oxychloride amorphous solid electrolytes for long-cycling all-solid-state lithium batteries
Shumin Zhang, Feipeng Zhao, Jiatang Chen, Jiamin Fu, Jing Luo, Sandamini H. Alahakoon, Lo‐Yueh Chang, Renfei Feng, Mohsen Shakouri, Jianwen Liang, Yang Zhao, Xiaona Li, Le He, Yining Huang, Tsun‐Kong Sham, Xueliang Sun
Abstract
Abstract Solid electrolyte is vital to ensure all-solid-state batteries with improved safety, long cyclability, and feasibility at different temperatures. Herein, we report a new family of amorphous solid electrolytes, xLi 2 O-MCl y (M = Ta or Hf, 0.8 ≤ x ≤ 2, y = 5 or 4). xLi 2 O-MCl y amorphous solid electrolytes can achieve desirable ionic conductivities up to 6.6 × 10 −3 S cm −1 at 25 °C, which is one of the highest values among all the reported amorphous solid electrolytes and comparable to those of the popular crystalline ones. The mixed-anion structural models of xLi 2 O-MCl y amorphous SEs are well established and correlated to the ionic conductivities. It is found that the oxygen-jointed anion networks with abundant terminal chlorines in xLi 2 O-MCl y amorphous solid electrolytes play an important role for the fast Li-ion conduction. More importantly, all-solid-state batteries using the amorphous solid electrolytes show excellent electrochemical performance at both 25 °C and −10 °C. Long cycle life (more than 2400 times of charging and discharging) can be achieved for all-solid-state batteries using the xLi 2 O-TaCl 5 amorphous solid electrolyte at 400 mA g −1 , demonstrating vast application prospects of the oxychloride amorphous solid electrolytes.