Summary: | Lithium-air batteries (LABs) continue to receive attention as a promising power source because they possess a high theoretical energy density of 3436 Wh L<sup>−1</sup>. However, the remaining Li<sub>2</sub>O<sub>2</sub> resulting from the irreversible decomposition of Li<sub>2</sub>O<sub>2</sub> during the charge process is one of the key challenges so as to address the deterioration of the cycling performance of LABs. In this study, we propose and report a redox-mediated polymer catalyst (RPC) as a cathode catalyst being composed of LiI and poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) with multi-wall carbon nanotubes (MWCNTs) as the cathode material. In the RPC, iodine molecules are chemically combined with the PVDF-HFP chain. The as-prepared RPC exhibits increased cycling performance by 194% and decreased overpotential by 21.1% at 0.1 mA cm<sup>−2</sup> compared to the sample without LiI molecules. Furthermore, these results suggest that the RPC consisting of a polymer chain and redox mediators will be extensively utilized as highly efficient catalysts of LABs.
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