First-principles computational insights into lithium battery cathode materials

Lithium-ion batteries (LIBs) are considered to be indispensable in modern society. Major advances in LIBs depend on the development of new high-performance electrode materials, which requires a fundamental understanding of their properties. First-principles calculations have become a powerful technique in developing new electrode materials for high-energy–density LIBs in terms of predicting and interpreting the characteristics and behaviors of electrode materials, understanding the charge/discharge mechanisms at the atomic scale, delivering rational design strategies for electrode materials, etc. In this review, we present an overview of first-principles calculation methods and highlight their valuable role in contemporary research on LIB cathode materials. This overview focuses on three LIB cathode scenarios, which are divided by their cationic/anionic redox mechanisms. Then, representative examples of rational cathode design based on theoretical predictions are presented. Finally, we present a personal perspective on the current challenges and future directions of first-principles calculations in LIBs. Graphical abstract