DICP OpenIR
Dual effects of water vapor on ceria-supported gold clusters
Li, Zhimin1; Li, Weili2; Abroshan, Hadi3; Ge, Qingjie2; Li, Gao1; Jin, Rongchao3
Source PublicationNANOSCALE
2018-04-14
ISSN2040-3364
DOI10.1039/c7nr09447g
Volume10Issue:14Pages:6558-6565
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
WOS SubjectChemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS KeywordPROBING DEFECT SITES ; CO OXIDATION ; AU-25 NANOCLUSTERS ; AU-25(SCH2CH2PH)(18) NANOCLUSTERS ; PERIMETER SITES ; NANOPARTICLES ; CATALYSIS ; ACTIVATION ; SURFACE ; OXIDE
AbstractAtomically precise nanocatalysts are currently being intensely pursued in catalysis research. Such nanocatalysts can serve as model catalysts for gaining fundamental insights into catalytic processes. In this work we report a discovery that water vapor provokes the mild removal of surface long-chain ligands on 25-atom Au-25(SC12H25)(18) nanoclusters in a controlled manner. Using the resultant Au-25(SC12H25)(18-x)/CeO2 catalyst and CO oxidation as a probe reaction, we found that the catalytic activity of cluster/CeO2 is enhanced from nearly zero conversion of CO (in the absence of water) to 96.2% (in the presence of 2.3 vol% H2O) at the same temperature (100 degrees C). The cluster catalysts exhibit high stability during the CO oxidation process under moisture conditions (up to 20 vol% water vapor). Water vapor plays a dual role in gold cluster-catalyzed CO oxidation. FT-IR and XPS analyses in combination with density functional theory (DFT) simulations suggest that the "-SC12H25" ligands are easier to be removed under a water vapor atmosphere, thus generating highly active sites. Moreover, the O-2(2-) peroxide species constitutes the active oxygen species in CO oxidation, evidenced by Raman spectroscopy analysis and isotope experiments on the CeO2 and cluster/CeO2. The results also indicate the perimeter sites of the interface of Au-25(SC12H25)(18-x)/CeO2 to be active sites for catalytic CO oxidation. The controlled exposure of active sites under mild conditions is of critical importance for the utilization of clusters in catalysis.
Language英语
WOS IDWOS:000429530400036
PublisherROYAL SOC CHEMISTRY
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Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/167215
Collection中国科学院大连化学物理研究所
Corresponding AuthorGe, Qingjie; Li, Gao
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, Dalian 116023, Peoples R China
3.Carnegie Mellon Univ, Dept Chem, 4400 5th Ave, Pittsburgh, PA 15213 USA
Recommended Citation
GB/T 7714
Li, Zhimin,Li, Weili,Abroshan, Hadi,et al. Dual effects of water vapor on ceria-supported gold clusters[J]. NANOSCALE,2018,10(14):6558-6565.
APA Li, Zhimin,Li, Weili,Abroshan, Hadi,Ge, Qingjie,Li, Gao,&Jin, Rongchao.(2018).Dual effects of water vapor on ceria-supported gold clusters.NANOSCALE,10(14),6558-6565.
MLA Li, Zhimin,et al."Dual effects of water vapor on ceria-supported gold clusters".NANOSCALE 10.14(2018):6558-6565.
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