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

Aykol, Muratahan; Kim, Soo; Hegde, Vinay I.; Kirklin, Scott; Wolverton, Chris

doi:10.1103/physrevmaterials.3.025402

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

Journal Article · 05 February 2019 · Physical Review Materials

DOI: https://doi.org/10.1103/physrevmaterials.3.025402 · OSTI ID:1544121

Aykol, Muratahan ^[1]; Kim, Soo ^[1]; Hegde, Vinay I. ^[1]; Kirklin, Scott ^[1]; Wolverton, Chris ^[1]

Northwestern Univ., Evanston, IL (United States)

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. Specifically, we tested around 180 combinations of elemental substitutions for the dodecahedral X sites and octahedral Y sites in the Li₃X₃Y₂O₁₂ 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) Li₃ garnets with respect to decomposition to other stable phases in the Open Quantum Materials Database in the respective four-dimensional Li-X-Y -O 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 Li3-garnet compounds and classify each for potential applications as an anode, cathode, or solid-state electrolyte to be used in LIBs. Finally, Li⁺ ion diffusivity is calculated for the representative Li₃Nd₃W₂O₁₂ model system. The results we present here are expected to serve as a guideline for designing new garnet oxides for Li-ion battery applications.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: National Institute of Standards and Technology (NIST); US Department of Commerce; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0015106

OSTI ID:: 1544121

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 2 Vol. 3; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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