Morphology effect of ceria supports on gold nanocluster catalyzed CO oxidation

The interfacial perimeter is generally viewed as the catalytically active site for a number of chemical reactions over oxide-supported nanogold catalysts. Here, well-defined CeO 2 nanocubes, nanorods and nanopolyhedra are chosen to accommodate atomically precise clusters ( e.g. Au 25 (PET) 18 ) to g...

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Published inNanoscale advances Vol. 3; no. 24; pp. 72 - 76
Main Authors Li, Zhimin, Zhang, Xinyu, Shi, Quanquan, Gong, Xia, Xu, Hui, Li, Gao
Format Journal Article
LanguageEnglish
Published RSC 07.12.2021
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Summary:The interfacial perimeter is generally viewed as the catalytically active site for a number of chemical reactions over oxide-supported nanogold catalysts. Here, well-defined CeO 2 nanocubes, nanorods and nanopolyhedra are chosen to accommodate atomically precise clusters ( e.g. Au 25 (PET) 18 ) to give different Au cluster-CeO 2 interfaces. TEM images show that Au particles of ∼1.3 nm are uniformly anchored on the ceria surface after annealing in air at 120 °C, which can rule out the size hierarchy of nanogold in CO oxidation studies. The gold nanoclusters are only immobilized on the CeO 2 (200) facet in Au 25 /CeO 2 -C, while they are selectively loaded on CeO 2 (002) and (111) in the Au 25 /CeO 2 -R and Au 25 /CeO 2 -P catalysts. X-ray photoelectron spectroscopy (XPS) and in situ infrared CO adsorption experiments clearly demonstrate that the gold species in the Au 25 /CeO 2 samples are similar and partially charged (Au δ + , where 0 < δ < 1). It is observed that the catalytic activity decreases in the order of Au/CeO 2 -R Au/CeO 2 -P > Au/CeO 4 -C in the CO oxidation. And the apparent activation energy over Au 25 /CeO 2 -C (60.5 kJ mol −1 ) is calculated to be about two-fold of that over the Au 25 /CeO 2 -R (28.6 kJ mol −1 ) and Au 25 /CeO 2 -P (31.3 kJ mol −1 ) catalysts. It is mainly tailored by the adsorbed [O] species on the ceria surface, namely, Au 25 /CeO 2 (002) and Au 25 /CeO 2 (111) which were more active than the Au 25 /CeO 2 (200) system in the CO oxidation. These insights at the molecular level may provide guidelines for the design of new oxide-supported nanogold catalysts for aerobic oxidations. The interfacial perimeter is generally viewed as the catalytically active site for a number of chemical reactions over oxide-supported nanogold catalysts.
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Z. L. and X. Z. contributed equally to this work.
ISSN:2516-0230
2516-0230
DOI:10.1039/d1na00680k