Abstract

Abstract Li-O2 batteries are one of the most promising next generation batteries due to their high energy density. However, they suffer from high charge overpotentials and severe side reactions. Here we report a bifunctional CeVO4 catalyst that not only lowers the charge potential by a photo-assisted mechanism, more importantly, promotes the efficient conversion of highly reactive oxidative intermediates to Li2O2, thus avoiding the oxidative decomposition of the electrolyte/cathode during discharge. Benefiting from its efficient electrocatalysis and the improved charging ability, 1.6x higher discharge capacity up to 6.14 mAh cm-2, low charge potential of 3.48 V and stable cycling performance are simultaneously achieved. Theoretical calculation and in-situ Raman spectra confirm the superior adsorptive and conversion ability of superoxide species by electrochemical reduction and chemical disproportionation reactions on the CeVO4 catalyst. These results indicate an effective strategy to break through the reported limitations of photo-assisted cathodes that are of a low electrocatalysis ability and limited discharge capacity. The significance of retaining a high energy density in photo-assisted Li-O2 batteries is highlighted.

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