Review: Application of the CALPHAD Approach and First-Principles Calculations to Electrode Materials in Li Ion Batteries

Design and development of novel electrode materials is one of several hot topics in studying Li ion battery. The CALPHAD (CALculation of PHAse Diagrams) approach enables calculation of stable and metastable phase equilibria, as well as thermodynamic properties for various materials, which has been applied to accelerate modern materials design in recent years. The traditional trial-and-error method is being replaced by the integration of CALPHAD with first-principles calculations, as well as empirical methods and key experiments. The CALPHAD approach and first-principles calculations have been proved to be a powerful tool in studying electrode materials, not only for calculation of phase equilibria and thermodynamic properties, but also for prediction of cell voltages in Li ion batteries, which allows for the design of future electrode materials with improved stability and efficiency. Examples of the cathode systems (Li-O, Li-Co-O and Li-Ni-O) and anode systems (Li-Sb and Li-Sn), which are studied by applying the CALPHAD approach and first-principles calculations, are presented.