Dual effects of water vapor on ceria-supported gold clusters
文献类型：期刊论文
| 作者 | Li, Zhimin2; Abroshan, Hadi3; Jin, Rongchao3; Li, Gao2; Li, Weili1; Ge, Qingjie1 |
| 刊名 | NANOSCALE
 |
| 出版日期 | 2018-04-14 |
| 卷号 | 10期号:14页码:6558-6565 |
| ISSN号 | 2040-3364 |
| DOI | 10.1039/c7nr09447g |
| 文献子类 | Article |
| 英文摘要 | Atomically 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. |
| WOS关键词 | PROBING DEFECT SITES ; CO OXIDATION ; AU-25 NANOCLUSTERS ; AU-25(SCH2CH2PH)(18) NANOCLUSTERS ; PERIMETER SITES ; NANOPARTICLES ; CATALYSIS ; ACTIVATION ; SURFACE ; OXIDE |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:000429530400036 |
| 出版者 | ROYAL SOC CHEMISTRY |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/167214]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Li, Gao; Ge, Qingjie |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, Dalian 116023, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 3.Carnegie Mellon Univ, Dept Chem, 4400 5th Ave, Pittsburgh, PA 15213 USA |
| 推荐引用方式 GB/T 7714 | Li, Zhimin,Abroshan, Hadi,Jin, Rongchao,et al. Dual effects of water vapor on ceria-supported gold clusters[J]. NANOSCALE,2018,10(14):6558-6565. |
| APA | Li, Zhimin,Abroshan, Hadi,Jin, Rongchao,Li, Gao,Li, Weili,&Ge, Qingjie.(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. |
入库方式： OAI收割
来源：大连化学物理研究所
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