Regulating interfacial active sites to improve peroxymonosulfate (PMS) activation efficiency is a hot topic in the heterogeneous catalysis field. In this study, we develop an inverted loading strategy to engineer asymmetric Mn-O-Ce sites for PMS activation. MnO@CeO prepared by loading CeO nanoparticles onto MnO nanorods exhibits the highest catalytic activity and stability, which is due to the formation of more oxygen vacancies (O) at the Mn-O-Ce sites, and the surface CeO layer effectively inhibits corrosion by preventing the loss of manganese ion active species into the solution. In situ characterizations and density functional theory (DFT) studies have revealed effective bimetallic redox cycles at asymmetric Mn-O-Ce active sites, which promote surface charge transfer, enhance the adsorption reaction activity of active species toward pollutants, and favor PMS activation to generate (•OH, SO, O and O) active species. This study provides a brand-new perspective for engineering the interfacial behavior of PMS activation.
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