High-Throughput Description of Infinite Composition–Structure–Property–Performance Relationships of Lithium–Manganese Oxide Spinel Cathodes

Lithium–manganese oxide based spinel is attractive as cathode materials in lithium ion batteries. A wide range of spinel solid solution can be directly sintered and result in different properties of identical compositions during the battery operation, making it extremely difficult to understand the intrinsic properties and evaluate the battery performance. In this work, a high-throughput computational framework combining ab initio calculations and a CALPHAD (Calculation of Phase Diagrams) approach is developed to systematically describe infinite composition–structure–property–performance relationships under sintered and battery states of spinel cathodes. Depending on composition and crystallography, various properties (physical, thermochemical, and electrochemical) relating key factors (cyclability, safety, and energy density) are quantitatively mapped. The overall performance is consequently evaluated and validated by key experiments. Finally, 4 V spinel cathodes with codoping of reasonable Li and vacanc...