Journal of the American Chemical Society · 2019 · 174 citations · 57 references
Natural SciencesChemical EngineeringChemistryCatalysisInorganic ChemistryNanomaterialsCatalyst CharacterizationCatalyst StabilityCatalytic MaterialsCoordination ChemistryMetal Oxide NanomaterialsNanocatalysisActive Site CharacterizationActive Site FormationCo OxidationLong-term StabilityMetal Oxide CatalystsMetal Oxide NanocatalystsNanostructured CatalystsOxidation
The construction of stable active site in nanocatalysts is of great importance but is a challenge in heterogeneous catalysis. Unexpectedly, coordination-unsaturated and atomically dispersed copper species were constructed and stabilized in a sintered copper–ceria catalyst through air-calcination at 800 °C. This sintered copper–ceria catalyst showed a very high activity for CO oxidation with a CO consumption rate of 6100 μmolCO·gCu–1·s–1 at 120 °C, which was at least 20 times that of other reported copper catalysts. Additionally, the excellent long-term stability was unbroken under the harsh cycled reaction conditions. Based on a comprehensive structural characterization and mechanistic study, the copper atoms with unsaturated coordination in the form of Cu1O3 were identified to be the sole active site, at which both CO and O2 molecules were activated, thus inducing remarkable CO oxidation activity with a very low copper loading (1 wt %).
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