Computational evaluation of new lithium-3 garnets for lithium-ion battery applications as anodes, cathodes, and solid-state electrolytes

Abstract

Solid-state lithium-ion batteries are expected to power the next-generation of electric vehicles as an integral part of safer, higher-performance energy storage technologies. Using high-throughput density functional theory calculations, combined with the Open Quantum Materials Database (OQMD), the authors explore a large chemical space of potential, new Li${}_{3}$X${}_{3}$Y${}_{2}$O${}_{12}$ compounds with the garnet crystal structure to identify material candidates that can serve as electrode or electrolyte components in such a solid-state system. Their virtual screening strategy is guided by thermodynamic rules, along with insights from Li-ion dynamics, and yields a list of new, computer-designed Li-3 garnets as the most promising candidates among the hundreds of possibilities in this material class. These ``computational discoveries'' are made available to the community for experimental validation and evaluation in solid-state battery applications.