Recent advances in understanding of the mechanism and control of LiO formation in aprotic Li-O batteries.

Aprotic Li-O batteries represent promising alternative devices for electrical energy storage owing to their extremely high energy densities. Upon discharge, insulating solid LiO forms on cathode surfaces, which is usually governed by two growth models, namely the solution model and the surface model. These LiO growth models can largely determine the battery performances such as the discharge capacity, round-trip efficiency and cycling stability. Understanding the LiO formation mechanism and controlling its growth are essential to fully realize the technological potential of Li-O batteries. In this review, we overview the recent advances in understanding the electrochemical and chemical processes that occur during the LiO formation. In the beginning, the oxygen reduction mechanisms, the identification of O/LiO intermediates, and their influence on the LiO morphology have been discussed. The effects of the discharge current density and potential on the LiO growth model have been subsequently reviewed. Special focus is then given to the prominent strategies, including the electrolyte-mediated strategy and the cathode-catalyst-tailoring strategy, for controlling the LiO growth pathways. Finally, we conclude by discussing the profound implications of controlling LiO formation for further development in Li-O batteries.