Computational understanding and multiscale simulation of secondary batteries

Secondary batteries are the most commercially viable and widely used energy storage devices owing to their portability, high-efficiency, and long service life. However, significant advancements in battery performance are required, in order to meet the growing demand of the emerging markets for higher energy density and better sustainability. This depends on an in-depth understanding of the working principles and updated materials of the batteries across multiple scales. In recent years, theoretical calculations have been widely employed for exploring the energy-storage mechanisms of various secondary batteries and assisting in the virtual screening of promising material candidates. This review primarily highlights the thermodynamic and kinetic applications of first-principles calculations, molecular dynamics, Monte Carlo method, high-throughput screening and machine learning in the development of two key battery materials (electrode and electrolyte) by summarizing recent progresses. It provides useful references and insights for future researches on the fundamental redox reactions and capacity decay mechanisms of secondary batteries, which are expected to facilitate accurate prediction of material properties, targeted design of material structure/composition, and accelerated development of high-performance secondary batteries.