期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 17, 页码 4642-4646出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201801103
关键词
aerobic oxidation; benzyl alcohol; palladium clusters; single atom catalysts; supported catalysts
资金
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117, 51232005]
- China Ministry of Science and Technology [0202801]
- Shenzhen Projects for Basic Research [KQCX20140521161756227]
- 973 Project [2014CB932400]
The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium-cerium oxide (Pd-1/CeO2) and hexapalladium cluster-cerium oxide (Pd-6/CeO2), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd-1/CeO2 shows extremely high catalytic activity with a TOF of 6739 h(-1) and satisfactory selectivity (almost 100% for benzaldehyde), while Pd-6/CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd-6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd-Ce perimeter.
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