Lithium‐Oxygen Chemistry at Well‐Designed Model Interface Probed by In Situ Spectroscopy Coupled with Theoretical Calculations

Abstract The aprotic lithium‐oxygen (Li‐O 2 ) battery has an extremely high theoretical specific energy and potentially provides a tantalizing solution to the renewable energy storage challenge encountered by contemporary and future societies. Nevertheless, the realization of practical Li‐O 2 batteries currently meets with substantial challenges that include, but are not limited to, low energy capability and short longevity. To address these obstacles, unveiling the reaction processes and degradation mechanisms of Li‐O 2 batteries is crucially important. Over recent years, the research paradigm of in situ spectroscopy coupled with theoretical calculations performed on well‐designed model interfaces, has proved to be indispensable for the fundamental study and performance optimization of various energy storage devices. In this contribution, first representative illustrations of this research paradigm are offered in the study of both primary and parasitic reactions of Li‐O 2 batteries, which significantly simplifies, but not degrade, the complex reaction conditions and decouples multiple processes occurring simultaneously in Li‐O 2 cells. Then, the perspective is provided on the remaining issues as well as uncertainties and discuss future research directions. Finally, wider research community is encouraged to tailor‐design versatile model interfaces to better bridge in situ spectroscopy and theoretical calculations for the research and development of better Li‐O 2 batteries and beyond.