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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U2 - 10.1039/c7ee01782k
DO - 10.1039/c7ee01782k
M3 - Article
AN - SCOPUS:85031498697
VL - 10
SP - 2201
EP - 2211
JO - Energy and Environmental Science
JF - Energy and Environmental Science
SN - 1754-5692
IS - 10
ER -