Material design of high-capacity Li-rich layered-oxide electrodes: Li2MnO3 and beyond

Soo Kim; Muratahan Aykol; Vinay I. Hegde; Zhi Lu; Scott Kirklin; Jason R. Croy; Michael M. Thackeray; Chris Wolverton

doi:10.1039/c7ee01782k

Material design of high-capacity Li-rich layered-oxide electrodes: Li₂MnO₃ and beyond

Soo Kim, Muratahan Aykol, Vinay I. Hegde, Zhi Lu, Scott Kirklin, Jason R. Croy, Michael M. Thackeray, Chris Wolverton^*

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

47 Scopus citations

Abstract

Lithium-ion batteries (LIBs) have been used widely in portable electronics, and hybrid-electric and all-electric vehicles for many years. However, there is a growing need to develop new cathode materials that will provide higher cell energy densities for advanced applications. Several candidates, including Li₂MnO₃-stabilized LiM′O₂ (M′ = Mn/Ni/Co) structures, Li₂Ru_0.75Sn_0.25O₃ (i.e., 3Li₂RuO₃-Li₂SnO₃), and disordered Li₂MoO₃-LiCrO₂ compounds can yield capacities exceeding 200 mA h g^-1, alluding to the constructive role that Li₂MO₃ (M⁴⁺) end-member compounds play in the electrochemistry of these systems. Here, we catalog the family of Li₂MO₃ compounds as active cathodes or inactive stabilizing agents using high-throughput density functional theory (HT-DFT). With an exhaustive search based on design rules that include phase stability, cell potential, resistance to oxygen evolution, and metal migration, we predict a number of new Li₂M_IO₃-Li₂M_IIO₃ active/inactive electrode pairs, in which M_I and M_II are transition- or post-transition metal ions, that can be tested experimentally for high-energy-density LIBs.

Original language	English (US)
Pages (from-to)	2201-2211
Number of pages	11
Journal	Energy and Environmental Science
Volume	10
Issue number	10
DOIs	https://doi.org/10.1039/c7ee01782k
State	Published - Oct 2017

ASJC Scopus subject areas

Environmental Chemistry
Renewable Energy, Sustainability and the Environment
Nuclear Energy and Engineering
Pollution

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@article{db4ec2efd4f246928e13bc086e51f0c8,

title = "Material design of high-capacity Li-rich layered-oxide electrodes: Li2MnO3 and beyond",

abstract = "Lithium-ion batteries (LIBs) have been used widely in portable electronics, and hybrid-electric and all-electric vehicles for many years. However, there is a growing need to develop new cathode materials that will provide higher cell energy densities for advanced applications. Several candidates, including Li2MnO3-stabilized LiM′O2 (M′ = Mn/Ni/Co) structures, Li2Ru0.75Sn0.25O3 (i.e., 3Li2RuO3-Li2SnO3), and disordered Li2MoO3-LiCrO2 compounds can yield capacities exceeding 200 mA h g-1, alluding to the constructive role that Li2MO3 (M4+) end-member compounds play in the electrochemistry of these systems. Here, we catalog the family of Li2MO3 compounds as active cathodes or inactive stabilizing agents using high-throughput density functional theory (HT-DFT). With an exhaustive search based on design rules that include phase stability, cell potential, resistance to oxygen evolution, and metal migration, we predict a number of new Li2MIO3-Li2MIIO3 active/inactive electrode pairs, in which MI and MII are transition- or post-transition metal ions, that can be tested experimentally for high-energy-density LIBs.",

author = "Soo Kim and Muratahan Aykol and Hegde, {Vinay I.} and Zhi Lu and Scott Kirklin and Croy, {Jason R.} and Thackeray, {Michael M.} and Chris Wolverton",

note = "Funding Information: S. Kim was supported by the Northwestern-Argonne Institution of Science and Engineering (NAISE). M. A. and Z. L. were supported by the Dow Chemical Company. S. Kirklin and C. W. were supported as part of the Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award No. DE-AC02-06CH11357). V. I. H. was supported by the National Scientific Foundation (NSF, DMR-1309957). Support from the Advanced Batteries Materials Research (BMR) Program, in particular David Howell and Tien Duong, of the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged by J. R. C. and M. M. T. 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 U.S. Department of Energy under Contract No. DE-AC02-05CH11231. S. Kim, M. A., V. I. H., and C. W. initially proposed the concept of performing HT-DFT calculations of Li2MO3 cathode structures and their related properties. V. I. H. and S. Kirklin helped setting up the calculations within the OQMD framework. S. Kim, M. A., and V. I. H. initially prepared the manuscript and figures with input from Z. L., J. R. C., M. M. T., and C. W. All authors contributed to the discussions and revision of the manuscript.",

year = "2017",

month = oct,

doi = "10.1039/c7ee01782k",

language = "English (US)",

volume = "10",

pages = "2201--2211",

journal = "Energy and Environmental Science",

issn = "1754-5692",

publisher = "Royal Society of Chemistry",

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TY - JOUR

T1 - Material design of high-capacity Li-rich layered-oxide electrodes

T2 - Li2MnO3 and beyond

AU - Kim, Soo

AU - Aykol, Muratahan

AU - Hegde, Vinay I.

AU - Lu, Zhi

AU - Kirklin, Scott

AU - Croy, Jason R.

AU - Thackeray, Michael M.

AU - Wolverton, Chris

N1 - Funding Information: S. Kim was supported by the Northwestern-Argonne Institution of Science and Engineering (NAISE). M. A. and Z. L. were supported by the Dow Chemical Company. S. Kirklin and C. W. were supported as part of the Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award No. DE-AC02-06CH11357). V. I. H. was supported by the National Scientific Foundation (NSF, DMR-1309957). Support from the Advanced Batteries Materials Research (BMR) Program, in particular David Howell and Tien Duong, of the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged by J. R. C. and M. M. T. 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 U.S. Department of Energy under Contract No. DE-AC02-05CH11231. S. Kim, M. A., V. I. H., and C. W. initially proposed the concept of performing HT-DFT calculations of Li2MO3 cathode structures and their related properties. V. I. H. and S. Kirklin helped setting up the calculations within the OQMD framework. S. Kim, M. A., and V. I. H. initially prepared the manuscript and figures with input from Z. L., J. R. C., M. M. T., and C. W. All authors contributed to the discussions and revision of the manuscript.

PY - 2017/10

Y1 - 2017/10

N2 - Lithium-ion batteries (LIBs) have been used widely in portable electronics, and hybrid-electric and all-electric vehicles for many years. However, there is a growing need to develop new cathode materials that will provide higher cell energy densities for advanced applications. Several candidates, including Li2MnO3-stabilized LiM′O2 (M′ = Mn/Ni/Co) structures, Li2Ru0.75Sn0.25O3 (i.e., 3Li2RuO3-Li2SnO3), and disordered Li2MoO3-LiCrO2 compounds can yield capacities exceeding 200 mA h g-1, alluding to the constructive role that Li2MO3 (M4+) end-member compounds play in the electrochemistry of these systems. Here, we catalog the family of Li2MO3 compounds as active cathodes or inactive stabilizing agents using high-throughput density functional theory (HT-DFT). With an exhaustive search based on design rules that include phase stability, cell potential, resistance to oxygen evolution, and metal migration, we predict a number of new Li2MIO3-Li2MIIO3 active/inactive electrode pairs, in which MI and MII are transition- or post-transition metal ions, that can be tested experimentally for high-energy-density LIBs.

AB - Lithium-ion batteries (LIBs) have been used widely in portable electronics, and hybrid-electric and all-electric vehicles for many years. However, there is a growing need to develop new cathode materials that will provide higher cell energy densities for advanced applications. Several candidates, including Li2MnO3-stabilized LiM′O2 (M′ = Mn/Ni/Co) structures, Li2Ru0.75Sn0.25O3 (i.e., 3Li2RuO3-Li2SnO3), and disordered Li2MoO3-LiCrO2 compounds can yield capacities exceeding 200 mA h g-1, alluding to the constructive role that Li2MO3 (M4+) end-member compounds play in the electrochemistry of these systems. Here, we catalog the family of Li2MO3 compounds as active cathodes or inactive stabilizing agents using high-throughput density functional theory (HT-DFT). With an exhaustive search based on design rules that include phase stability, cell potential, resistance to oxygen evolution, and metal migration, we predict a number of new Li2MIO3-Li2MIIO3 active/inactive electrode pairs, in which MI and MII are transition- or post-transition metal ions, that can be tested experimentally for high-energy-density LIBs.

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