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(Invited) High-Throughput DFT Thermochemistry Applied to the Design of Cathode Coatings Forlithium-Ion Batteries

Wednesday, 1 June 2016: 08:30
Indigo 202 A (Hilton San Diego Bayfront)
C. Wolverton (Northwestern University)
We present a high-throughput (HT) density functional theory (DFT) based framework to identify new functional coatings that can suppress cathode degradation in Li-ion batteries. This HT framework is based on reaction models that describe the thermodynamic and electrochemical stabilities and acid-scavenging capabilities of oxide materials. Using the framework, we search for coatings with different functionalities including physical barriers, hydrofluoric acid (HF) barriers and HF scavengers, by screening more than 130,000 candidate oxide materials. Employing two alternative material selection methods, namely, weighted-sum and rank aggregation multi-objective optimization, we predict new promising physical and HF-barrier coating materials such as WO3, LiAl5O8, ZrP2O7, Hf2P2O9, TaPO5, CaSn4(PO4)6, and new or under-explored HF-scavengers such as Sc2O3, Li2CaGeO4, Li3NbO4, TaBO4, LiBO2, Mg3(BO3)2, Ca5(BO3)3F, Ca2Ta2O7 and Li2MgSiO4. Using principal component analysis, we show that the the likelihood of discovery of effective HF-scavenger coatings is highest in silicates and borates among all oxides. We further present a new HT design strategy where thermodynamically optimal HF-scavenger coatings for a given cathode material can be found by (i) incorporating the cathode material itself in the chemical space, (ii) evaluating the cathode-coating reactivity, and (iii) monitoring cathode reactivity in electrochemical (charge and discharge) and HF-attack reactions. Examples of such optimal coatings we found include Li2SrSiO4, Li2CaSiO4 and CaIn2O4 coatings for the layered LiCoO2 and Li2GeO3, Li2TiSiO5, Li4NiTeO6, Ca2Mn3O8, and Li2MnO3 for the spinel LiMn2O4 cathodes. These candidate coating materials have the potential to prolong the cycle-life of lithium-ion batteries and surpass the performance of common coating technologies based on conventional materials such as Al2O3, ZnO, MgO or ZrO2. This work was performed in collaboration with Muratahan Aykol, Soo Kim, Vinay I. Hegde, David Snydacker, Zhi Lu, Shiqiang Hao, Scott Kirklin, and Dane Morgan.