Using First‐Principles Calculations for the Advancement of Materials for Rechargeable Batteries

Abstract Rechargeable batteries have been regarded as leading candidates for energy storage systems to satisfy soaring energy demands and ensure efficient energy use, and intensive efforts have thus been focused on enhancing their energy densities and power capabilities. First‐principles calculations based on quantum mechanics have played an important role in obtaining a fundamental understanding of battery materials, thus providing insights for material design. In this feature article, the theoretical approaches used to determine key battery properties, such as the voltage, phase stability, and ion‐diffusion kinetics, are reviewed. Moreover, the recent contribution of first‐principles calculations to the interpretation of complicated experimental characterization measurements on battery materials, such as those obtained using X‐ray absorption spectroscopy, electron energy‐loss spectroscopy, nuclear magnetic resonance spectroscopy, and transmission electron microscopy, are introduced. Finally, perspectives are provided on the research direction of first‐principles calculations for the development of advanced batteries, including the further development of theories that can accurately describe the dissolved species, amorphous phases, and surface reactions that are integral to the operation of future battery systems beyond Li‐ion batteries.