Enhanced Oxygen Activation on Atomically Dispersed Au Catalyst with Dual Active Sites for Room-Temperature Formaldehyde Oxidation

Formaldehyde (HCHO) is known to be a hazardous indoor air pollutant. Noble metal catalysts offer a feasible approach for the indoor HCHO decomposition. Oxygen activation via a noble metal such as gold plays a critical role in realizing total HCHO oxidation, but then it is vague how different-sized noble metals function synergistically on oxygen activation. Here, an Au/CeO2 catalyst with atomically dispersed Au (Au/CeO2-550) was successfully prepared through the thermal aging treatment, and a synergistic mechanism for the HCHO oxidation reaction involving co-loaded of single Au atoms and Au nanoclusters on CeO2 was revealed. Strikingly, the HCHO oxidation performance of the obtained Au/CeO2-550 catalyst at room temperature was significantly greater than that of other Au/CeO2 catalysts, which was attributed to a concerted catalysis mechanism of the individual Au atoms and nanoclusters. The surface oxygen species of CeO2 activated by single Au atoms can promptly transform HCHO to dioxymethylene species, while Au nanoclusters well adsorb and activate molecular oxygen to oxidize the dioxymethylene into formate, which is further oxidized into carbonates, and carbonate is eventually decomposed into CO2 and H2O. This synergy results in enhanced HCHO oxidation at surface sites between neighboring single Au atoms and Au nanoclusters.

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