Current-Dependent Morphologies of Insulating Electrodeposits in Li–O2 Batteries Controlled by Coupled Ion-Electron Transfer Kinetics

Lithium–oxygen batteries (Li–O 2 ) present a compelling prospect for the next generation of batteries owing to their exceptionally high theoretical energy density. However, the performance of Li–O 2 batteries remains limited by the formation of insulating oxides covering the gas electrode, leading to low capacity or even unexpected sudden death. Existing mathematical models using Butler–Volmer kinetics exhibit uncertainties and inaccuracies in predicting the voltage responses and the morphological evolution of the insulating oxides. In this study, we incorporate coupled ion-electron transfer theory with a phase-field model to enable consistent predictions of the voltage curves, oxide morphologies, and roles of solvation energy. This study provides a valuable predictive tool for the predictive design of electrolytes and electrodes for batteries forming insulating products.