Lithium–air batteries (LABs) possess the highest energy density among all energy storage systems, and have drawn widespread interest in academia and industry. However, many arduous challenges are still to be conquered, one of them is Li
2CO
3, which is a
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Lithium–air batteries (LABs) possess the highest energy density among all energy storage systems, and have drawn widespread interest in academia and industry. However, many arduous challenges are still to be conquered, one of them is Li
2CO
3, which is a ubiquitous product in LABs. It is inevitably produced but difficult to decompose; therefore, Li
2CO
3 is perceived as the “Achilles’ heel of LABs”. Among various approaches to addressing the Li
2CO
3 issue, developing Li
2CO
3-decomposing redox mediators (RMs) is one of the most convenient and versatile, because they can be electrochemically oxidized at the gas cathode surface, then they diffuse to the solid-state products and chemically oxidize them, recovering the RMs to a pristine state and avoiding solid-state catalysts’ contact instability with Li
2CO
3. Furthermore, because of their function mechanism, they can double as catalysts for Li
2O
2/LiOH decomposition, which are needed in LABs/LOBs anyway regardless of Li
2CO
3 incorporation due to the sluggish kinetics of oxygen reduction/evolution reactions. This review summarizes the progress in Li
2CO
3-decomposing RMs, including halides, metal–chelate complexes, and metal-free organic compounds. The insights into and discrepancies in the mechanisms of Li
2CO
3 decomposition and corresponding catalysis processes are also discussed.
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