A review of rechargeable aprotic lithium–oxygen batteries based on theoretical and computational investigations

Abstract

Rechargeable lithium–oxygen (Li–O₂) batteries with ultrahigh theoretical energy density have attracted great attention as energy storage and conversion devices. However, due to the insoluble-insulating nature of the discharge product (Li₂O₂) and the high activity of the superoxide intermediate and Li-metal anode, the practical performance of aprotic Li–O₂ batteries, as a type of mostly studied and developed Li–O₂ battery, is greatly lower than expected. In recent years, theoretical calculations from both density functional theory (DFT) and molecular dynamic (MD) simulation have greatly contributed to understanding the reaction mechanisms and designing efficient materials for aprotic Li–O₂ batteries at the atomic scale. In this review, the recent advances in theoretical and computational investigations on aprotic Li–O₂ batteries from the Li₂O₂ growth/morphology, catalytic reaction kinetics, electrolytes and anode stability have been summarized and discussed, and the challenges, perspectives and future research directions have been proposed.