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 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.
Original language | English (US) |
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Article number | 025402 |
Journal | Physical Review Materials |
Volume | 3 |
Issue number | 2 |
DOIs | |
State | Published - Feb 6 2019 |
Funding
The authors acknowledge funding from the following sources: The electrochemical stability window and diffusivity calculations were supported by the financial assistance Award No. 70NANB14H012 from the US Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). The OQMD stability calculations were supported by the Department of Energy, Grant No. DE-SC0015106. The construction of the high-throughput framework was supported as part of the Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences (Award No. DE-AC02-06CH11357). This research was supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.
ASJC Scopus subject areas
- General Materials Science
- Physics and Astronomy (miscellaneous)