The aprotic lithium-oxygen (Li-O2) batteries are receiving intense research interest in virtue of their ultra-high theoretical specific energy. However, current Li-O2 batteries are sufferring from severe barriers, such as sluggish reaction kinetics and undesired parasitic reactions. Recently, molecular catlysts, i.e., redox mediators (RMs), have been explored to catalyze the oxygen electrochemistry in Li-O2 batteries and are regarded as an advanced solution. To fully unlock the capability of Li-O2 batteries, an in-depth understanding of the catalytic mechanisms of RMs is necessary. In this review, we summarize the working principles of RMs and their selection criteria, highlight the recent significant progress of RMs, and discuss the critical scientific and technical challenges on the design of efficient RMs for next-generation Li-O2 batteries.

The highly efficient bifunctional electrocatalytic activity of Co9S8@CPNs was confirmed by experiments and DFT calculations in aprotic Li–O2 batteries for the first time.

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