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

Muratahan Aykol, Soo Kim, Vinay I. Hegde, Scott Kirklin, and Chris Wolverton
Phys. Rev. Materials 3, 025402 – Published 6 February 2019
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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 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 LiXYO 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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  • Received 20 January 2018
  • Revised 10 November 2018

DOI:https://doi.org/10.1103/PhysRevMaterials.3.025402

©2019 American Physical Society

Physics Subject Headings (PhySH)

  1. Research Areas
  1. Physical Systems
Condensed Matter, Materials & Applied Physics

Authors & Affiliations

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

  • Department of Materials Science and Engineering, 2220 Campus Drive, Evanston Illinois, USA

  • *Present Address: Toyota Research Institute, Los Altos California, USA.
  • Present Address: Robert Bosch Research and Technology Center, Cambridge Massachusetts, USA.
  • Author to whom correspondence should be addressed: c-wolverton@northwestern.edu

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Issue

Vol. 3, Iss. 2 — February 2019

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