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, LiAl5O8and ZrP2O7and hydrofluoric-acid scavengers such as Sc2O3, Li2CaGeO4, LiBO2, Li3NbO4, Mg3(BO3)2and Li2MgSiO4. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li2SrSiO4, Li2CaSiO4and CaIn2O4for the layered LiCoO2, and Li2GeO3, Li4NiTeO6and Li2MnO3for the spinel LiMn2O4cathodes. 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.
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Muratahan
authors.initials: M
authors.lastname: Aykol
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Soo
authors.initials: S
authors.lastname: Kim
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Vinay I
authors.initials: VI
authors.lastname: Hegde
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: David
authors.initials: D
authors.lastname: Snydacker
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Zhi
authors.initials: Z
authors.lastname: Lu
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Shiqiang
authors.initials: S
authors.lastname: Hao
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: Scott
authors.initials: S
authors.lastname: Kirklin
authors.affiliation: Department of Materials Science and Engineering, University of Wisconsin, Madison, Wisconsin 53706, USA.
authors.forename: Dane
authors.identifier: 0000-0002-4911-0046
authors.initials: D
authors.lastname: Morgan
authors.affiliation: Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA.
authors.forename: C
authors.initials: C
authors.lastname: Wolverton