The interfacial oxygen-defective sites of oxide-supported metal catalysts are generally regarded as active centers in diverse redox reactions. Identification of their structure-property relationship at the atomic scale is of great importance but challenging. Herein, a series of La-doped three-dimensionally ordered macroporous CeO (3D-CeLaO) were synthesized and applied as supports for Pt nanoparticles. The pieces of evidence from a suite of in-situ/ex-situ characterizations and theoretical calculations revealed that the La-mono-substituted La-□(-Ce) sites (where □ represents an oxygen vacancy) exhibited superior charge transfer ability, behaving as trapping centers for Pt nanoparticles. The resulting interfacial Pt/La-□(-Ce) sites served as the reversible active species in the aerobic oxidation of 5-hydroxymethylfurfural to boost catalytic performance by simultaneously promoting oxygen activated capacity and the cleavage of O-H/C-H bonds of adsorbed hydroxymethyl groups. Consequently, the Pt/3D-CeLaO catalyst possessing the highest number of Pt/La-□(-Ce) sites showed the best catalytic performance with 99.6% yield to 2,5-furandicarboxylic acid in 10 h. These results offer more insights into the promoting mechanism of interfacial oxygen-defective sites for the liquid-phase aerobic oxidation of aldehydes and alcohols.
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