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CO Oxidation Catalyzed by Oxide-Supported Au-25(SR)(18) Nanoclusters and Identification of Perimeter Sites as Active Centers
Nie, Xiaotao1,3; Qian, Huifeng2; Ge, Qingjie1; Xu, Hengyong1; Jin, Rongchao2
关键词Au-25(Sr)(18) Nanocluster Supported Catalyst Co Oxidation Water Vapor Pretreatment Temperature
刊名ACS NANO
2012-07-01
DOI10.1021/nn301019f
6期:7页:6014-6022
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
类目[WOS]Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
研究领域[WOS]Chemistry ; Science & Technology - Other Topics ; Materials Science
关键词[WOS]PRECISE GOLD NANOCLUSTERS ; LOW-TEMPERATURE OXIDATION ; CARBON-MONOXIDE ; AU-25 CLUSTERS ; AU CATALYSTS ; NANOPARTICLES ; SIZE ; OXYGEN ; TIO2 ; SPECTROSCOPY
英文摘要In this work, we explore the catalytic application of atomically monodisperse, thiolate-protected Au-25(SR)(18) (where R = CH2CH2Ph) nanoclusters supported on oxides for CO oxidation. The solution phase nanoclusters were directly deposited onto various oxide supports (including TiO2, CeO2, and Fe2O3), and the as-prepared catalysts were evaluated for the CO oxidation reaction in a fixed bed reactor. The supports exhibited a strong effect, and the Au-25(SR)(18)/CeO2 catalyst was found to be much more active than the others. Interestingly, O-2 pretreatment of the catalyst at 150 degrees C for 1.5 h significantly enhanced the catalytic activity. Since this pretreatment temperature is well below the thiolate desorption temperature (similar to 200 degrees C), the thiolate ligands should remain on the Au-25 cluster surface, indicating that the CO oxidation reaction is catalyzed by intact Au-25(SR)(18)/CeO2. We further found that increasing the O-2 pretreatment temperature to 250 degrees C (above the thiolate desorption temperature) did not lead to any further increase in activity at all reaction temperatures from room temperature to 100 degrees C. These results are in striking contrast with the common thought that surface thiolates must be removed-as is often done in the literature work-before the catalyst can exert high catalytic activity. The 150 degrees C O-2-pretreated Au-25(SR)(18)/CeO2 catalyst offers similar to 94% CO conversion at 80 degrees C and similar to 100% conversion at 100 degrees C. The effect of water vapor on the catalytic performance is also investigated. Our results imply that the perimeter sites of the interface of Au-25(SR)(18)/CeO2 should be the active centers. The intact structure of the Au-25(SR)(18) catalyst in the CO oxidation process allows one to gain mechanistic insight into the catalytic reaction.
语种英语
WOS记录号WOS:000306673800030
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/143039
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
3.Chinese Acad Sci, Grad Univ, Beijing 100049, Peoples R China
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GB/T 7714
Nie, Xiaotao,Qian, Huifeng,Ge, Qingjie,et al. CO Oxidation Catalyzed by Oxide-Supported Au-25(SR)(18) Nanoclusters and Identification of Perimeter Sites as Active Centers[J]. ACS NANO,2012,6(7):6014-6022.
APA Nie, Xiaotao,Qian, Huifeng,Ge, Qingjie,Xu, Hengyong,&Jin, Rongchao.(2012).CO Oxidation Catalyzed by Oxide-Supported Au-25(SR)(18) Nanoclusters and Identification of Perimeter Sites as Active Centers.ACS NANO,6(7),6014-6022.
MLA Nie, Xiaotao,et al."CO Oxidation Catalyzed by Oxide-Supported Au-25(SR)(18) Nanoclusters and Identification of Perimeter Sites as Active Centers".ACS NANO 6.7(2012):6014-6022.
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