Application of first-principles calculations to the design of rechargeable Li-batteries

Abstract Rechargeable Li batteries consist of an anode, electrolyte, and cathode. The cathode is typically an oxide that intercalates Li at very low chemical potential ensuring a large open-cell voltage for the battery. We show how first-principles pseudopotential calculations can be used to predict the intercalation voltage for these materials. By means of a series of computational experiments on virtual structures, we identify the parameters that are important in determining the intercalation voltage of a compound. We found that Li intercalation causes significant electron transfer to the oxygen ions in the structure. Results are presented for LiTiO 2 , LiVO 2 , LiMnO 2 , LiCoO 2 , LiNiO 2 , and LiZnO 2 .