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Oxygen reduction reaction (ORR) plays a pivotal role in advanced electrochemical energy conversion devices. However, the ORR conversion efficiency is extremely limited. The major obstacles originate from the adsorption and activation of O2 on the electrode surface. A novel nanocomposite catalyst, photosensitizers (PS) meso-tetraphenylporphyrin iron(III) chloride (FePcCl)/NiCoFe-layered double hydroxides (NiCoFe-LDHs) is designed in this study. Herein, owing to excellent oxygen molecules activation ability and remarkable illumination absorption feature, FePcCl/NiCoFe-LDHs is employed to uncover the relationship between the intrinsic ORR activity and PS behaviour. Interestingly, the reaction mechanism of singlet 1O2 is proposed owing to the combination of electrochemical ORR catalysed via LDHs and PS. The boosted cathodic ORR properties exhibit singlet 1O2 dependent response arising from the synergistic effect to selectively produce active intermediates in alkaline medium. This work imparts the promising new mechanism about the high 4-electron ORR selectivity via material design, which will guide the development of photo-assisted energy conversion devices.
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