Rapid Hierarchical Screening for Promising Ternary and Quaternary Inorganic Solid-State Electrolytes
Xiaojun Zhao, Songzhao Duan, Binghui Zhou, Zhengyang Gao, Ian D. Gates, Weijie Yang
Abstract
All-solid-state Li-ion batteries are expected to solve the safety problems of traditional liquid electrolyte batteries and have received widespread attention. However, the low ionic conductivity and poor interfacial stability of electrolytes are the two factors hindering the application of all-solid-state batteries. Herein, we performed a fast and accurate hierarchical screening of 16,205 Li-containing compounds obtained from the Materials Project database to search for promising inorganic solid-state electrolytes (ISSEs). Thermodynamic stability, electronic insulation, electrochemical stability, and ionic conductivity were analyzed using density functional theory calculations combined with grand potential phase diagram (GPPD) analysis and ab initio molecular dynamics (AIMD) simulations. After screening, Li3AlF6 and Li4ZrF8 appeared to be potential solid-electrolyte materials due to their high Li-ion conductivity (0.991 and 0.477 mS/cm at room temperature, respectively) and robust interfacial stability with cathodes. The use of Li3AlF6 as a promising solid electrolyte is consistent with the previous literature, indicating the reliability of this work. In addition, the robust stability of the Li4ZrF8/LiCoO2 interface structure at 300 K illustrates the advantages of Li4ZrF8 as an electrolyte material.