High-throughput computational design of cathode coatings for Li-ion batteries

Muratahan Aykol; Soo Kim; Vinay I. Hegde; David Snydacker; Zhi Lu; Shiqiang Hao; Scott Kirklin; Dane Morgan; C. Wolverton

doi:10.1038/ncomms13779

High-throughput computational design of cathode coatings for Li-ion batteries

Muratahan Aykol, Soo Kim, Vinay I. Hegde, David Snydacker, Zhi Lu, Shiqiang Hao, Scott Kirklin, Dane Morgan, C. Wolverton^*

^*Corresponding author for this work

Materials Science and Engineering

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

148 Scopus citations

Abstract

Cathode degradation is a key factor that limits the lifetime of Li-ion batteries. To identify functional coatings that can suppress this degradation, we present a high-throughput density functional theory based framework which consists of reaction models that describe thermodynamic and electrochemical stabilities, and acid-scavenging capabilities of materials. Screening more than 130,000 oxygen-bearing materials, we suggest physical and hydrofluoric-acid barrier coatings such as WO₃, LiAl₅O₈ and ZrP₂O₇ and hydrofluoric-acid scavengers such as Sc₂O₃, Li₂CaGeO₄, LiBO₂, Li₃NbO₄, Mg₃ (BO₃)₂ and Li₂MgSiO₄. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li₂ SrSiO₄, Li₂CaSiO₄ and CaIn₂O₄ for the layered LiCoO₂, and Li₂GeO₃, Li₄NiTeO₆ and Li₂MnO₃ for the spinel LiMn₂O₄ cathodes. These coating materials have the potential to prolong the cycle-life of Li-ion batteries and surpass the performance of common coatings based on conventional materials such as Al₂O₃, ZnO, MgO or ZrO₂.

Original language	English (US)
Article number	13779
Journal	Nature communications
Volume	7
DOIs	https://doi.org/10.1038/ncomms13779
State	Published - Dec 14 2016

Funding

S. Kim was supported by Northwestern-Argonne Institute of Science and Engineering (NAISE). V.I.H. was supported by the National Science Foundation through grant DMR-1309957. S. Kirklin (OQMD calculations and qmpy software) was supported by the Center for Electrical Energy Storage: Tailored Interfaces, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. 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.

ASJC Scopus subject areas

General Physics and Astronomy
General Chemistry
General Biochemistry, Genetics and Molecular Biology

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title = "High-throughput computational design of cathode coatings for Li-ion batteries",

abstract = "Cathode degradation is a key factor that limits the lifetime of Li-ion batteries. To identify functional coatings that can suppress this degradation, we present a high-throughput density functional theory based framework which consists of reaction models that describe thermodynamic and electrochemical stabilities, and acid-scavenging capabilities of materials. Screening more than 130,000 oxygen-bearing materials, we suggest physical and hydrofluoric-acid barrier coatings such as WO3, LiAl5O8 and ZrP2O7 and hydrofluoric-acid scavengers such as Sc2O3, Li2CaGeO4, LiBO2, Li3NbO4, Mg3 (BO3)2 and Li2MgSiO4. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li2 SrSiO4, Li2CaSiO4 and CaIn2O4 for the layered LiCoO2, and Li2GeO3, Li4NiTeO6 and Li2MnO3 for the spinel LiMn2O4 cathodes. These coating materials have the potential to prolong the cycle-life of Li-ion batteries and surpass the performance of common coatings based on conventional materials such as Al2O3, ZnO, MgO or ZrO2.",

author = "Muratahan Aykol and Soo Kim and Hegde, {Vinay I.} and David Snydacker and Zhi Lu and Shiqiang Hao and Scott Kirklin and Dane Morgan and C. Wolverton",

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AU - Hao, Shiqiang

AU - Kirklin, Scott

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AU - Wolverton, C.

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N2 - Cathode degradation is a key factor that limits the lifetime of Li-ion batteries. To identify functional coatings that can suppress this degradation, we present a high-throughput density functional theory based framework which consists of reaction models that describe thermodynamic and electrochemical stabilities, and acid-scavenging capabilities of materials. Screening more than 130,000 oxygen-bearing materials, we suggest physical and hydrofluoric-acid barrier coatings such as WO3, LiAl5O8 and ZrP2O7 and hydrofluoric-acid scavengers such as Sc2O3, Li2CaGeO4, LiBO2, Li3NbO4, Mg3 (BO3)2 and Li2MgSiO4. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li2 SrSiO4, Li2CaSiO4 and CaIn2O4 for the layered LiCoO2, and Li2GeO3, Li4NiTeO6 and Li2MnO3 for the spinel LiMn2O4 cathodes. These coating materials have the potential to prolong the cycle-life of Li-ion batteries and surpass the performance of common coatings based on conventional materials such as Al2O3, ZnO, MgO or ZrO2.

AB - Cathode degradation is a key factor that limits the lifetime of Li-ion batteries. To identify functional coatings that can suppress this degradation, we present a high-throughput density functional theory based framework which consists of reaction models that describe thermodynamic and electrochemical stabilities, and acid-scavenging capabilities of materials. Screening more than 130,000 oxygen-bearing materials, we suggest physical and hydrofluoric-acid barrier coatings such as WO3, LiAl5O8 and ZrP2O7 and hydrofluoric-acid scavengers such as Sc2O3, Li2CaGeO4, LiBO2, Li3NbO4, Mg3 (BO3)2 and Li2MgSiO4. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li2 SrSiO4, Li2CaSiO4 and CaIn2O4 for the layered LiCoO2, and Li2GeO3, Li4NiTeO6 and Li2MnO3 for the spinel LiMn2O4 cathodes. These coating materials have the potential to prolong the cycle-life of Li-ion batteries and surpass the performance of common coatings based on conventional materials such as Al2O3, ZnO, MgO or ZrO2.

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High-throughput computational design of cathode coatings for Li-ion batteries

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