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

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 WO, LiAlO and ZrPO and hydrofluoric-acid scavengers such as ScO, LiCaGeO, LiBO, LiNbO, Mg(BO) and LiMgSiO. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as LiSrSiO, LiCaSiO and CaInO for the layered LiCoO, and LiGeO, LiNiTeO and LiMnO for the spinel LiMnO 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 AlO, ZnO, MgO or ZrO.