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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Chemistry
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Abstract 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.
AbstractList 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.
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.
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.
Author Shi, Quanquan
Li, Zhimin
Zhang, Xinyu
Gong, Xia
Xu, Hui
Li, Gao
AuthorAffiliation Chinese Academy of Sciences
Inner Mongolia Agricultural University
State Key Laboratory of Catalysis
College of Science
Dalian Institute of Chemical Physics
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Z. L. and X. Z. contributed equally to this work.
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Snippet 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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StartPage 72
SubjectTerms Chemistry
Title Morphology effect of ceria supports on gold nanocluster catalyzed CO oxidation
URI https://search.proquest.com/docview/2716936896
https://pubmed.ncbi.nlm.nih.gov/PMC9417965
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