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CO Oxidation Catalyzed by Single Gold Atoms Supported on Aluminum Oxide Clusters
Li, Zi-Yu1,2; Yuan, Zhen1,2; Li, Xiao-Na1; Zhao, Yan-Xia1; He, Sheng-Gui1
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2014-10-08
卷号136期号:40页码:14307-14313
ISSN号0002-7863
DOI10.1021/ja508547z
英文摘要The single gold atom doped aluminum oxide clusters AuAl3O3+, AuAl3O4+, and AuAl3O5+ have been prepared and mass-selected to react with CO, O-2, and mixtures of CO and O2 in an ion trap reactor under thermal collision conditions. The reactions have been characterized by mass spectrometry with isotopic substitution (O-16(2) -> O-18(2)) and density functional theory calculations. The AuAl3O5+ cluster can oxidize two CO molecules consecutively to form AuAl3O4+ and then AuAl3O3+, the latter of which can react with one O-2 molecule to regenerate AuAl3O5+. The (AuAl3O3+)-O-16 ions interact with a mixture of (CO)-O-16 and O-18(2) to produce the fully substituted O-18 species (AuAl3O3-5+)-O-18, which firmly identifies a catalytic cycle for CO oxidation by O-2. The oxidation catalysis is driven by electron cycling primarily through making and breaking a goldaluminum chemical bond. To the best of our knowledge, this is the first identification of catalytic CO oxidation by O-2 mediated with gas-phase cluster catalysts with single-noble-metal atoms, which serves as an important step to understand single-atom catalysis at strictly a molecular level.
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000343026700052
内容类型期刊论文
源URL[http://ir.iccas.ac.cn/handle/121111/51575]  
专题中国科学院化学研究所
通讯作者Li, Xiao-Na
作者单位1.Chinese Acad Sci, Beijing Natl Lab Mol Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Li, Zi-Yu,Yuan, Zhen,Li, Xiao-Na,et al. CO Oxidation Catalyzed by Single Gold Atoms Supported on Aluminum Oxide Clusters[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2014,136(40):14307-14313.
APA Li, Zi-Yu,Yuan, Zhen,Li, Xiao-Na,Zhao, Yan-Xia,&He, Sheng-Gui.(2014).CO Oxidation Catalyzed by Single Gold Atoms Supported on Aluminum Oxide Clusters.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,136(40),14307-14313.
MLA Li, Zi-Yu,et al."CO Oxidation Catalyzed by Single Gold Atoms Supported on Aluminum Oxide Clusters".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 136.40(2014):14307-14313.
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