Abstract
In this work, we explore a set of new garnet oxide structures that can be used as an anode, cathode or solid-electrolyte in lithium-ion batteries (LIBs) using high-throughput density functional theory. We tested around 180 combinations of elemental substitutions for the dodecahedral sites and octahedral sites in the type garnet structure and identified 19 stable (i.e., on the convex hull) and 11 nearly stable (i.e., within 50 meV/atom of the convex hull) garnets with respect to decomposition to other stable phases in the Open Quantum Materials Database in the respective four-dimensional chemical spaces. Our high-throughput screening strategy allows us to elucidate rules for garnet stability in terms of the ionic radii of the constituent elements. We evaluated the electrochemical window of these new, stable/nearly stable -garnet compounds and classify each for potential applications as an anode, cathode, or solid-state electrolyte to be used in LIBs. Finally, ion diffusivity is calculated for the representative model system. The results we present here are expected to serve as a guideline for designing new garnet oxides for Li-ion battery applications.
- Received 20 January 2018
- Revised 10 November 2018
DOI:https://doi.org/10.1103/PhysRevMaterials.3.025402
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