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Attaining high reversibility of electrodes and electrolyte is essential forthe longevity of secondary batteries. Rechargeable zinc-air batteries (RZABs),however, encounter drastic irreversible changes in the zinc anodes and aircathodes during cycling. To uncover the mechanisms of reversibility loss inRZABs, we investigate the evolution of zinc anode, alkaline electrolyte, andair electrode through experiments and first-principles calculations. Morphologydiagrams of zinc anodes under versatile operating conditions reveal that thenano-sized mossy zinc dominates the later cycling stage. Such anodic change isinduced by the increased zincate concentration due to hydrogen evolution, whichis catalyzed by the mossy structure and results in oxide passivation onelectrodes, and eventually leads to low true Coulombic efficiencies and shortlifespans of batteries. Inspired by these findings, we finally present a novelovercharge-cycling protocol to compensate the Coulombic efficiency loss causedby hydrogen evolution and significantly extend the battery life.

Decoding the Mechanisms of Reversibility Loss in Rechargeable Zinc-Air Batteries