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题名: Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines
作者: Chen, Haijun1, 2;  Liu, Chao3;  Wang, Min1;  Zhang, Chaofeng1;  Luo, Nengchao1, 2;  Wang, Yehong1;  Abroshan, Hadi4;  Li, Gao3;  Wang, Feng1
关键词: gold nanoclusters ;  Au-25 ;  photocatalysis ;  selective organic transformation ;  benzylamine oxidation
刊名: ACS CATALYSIS
发表日期: 2017-05-01
DOI: 10.1021/acscatal.6b03509
卷: 7, 页:3632-3638
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: This work demonstrates the synthesis of an efficient photocatalyst, Au-25(PPh3)(10)Cl-2(SC3H6SiO3)(5)/TiO2, for selective oxidation of amines to imines. The photocatalyst is prepared via hydrolysis of Au-25(PPh3)(10)Cl-2[(SC3H6Si(OC2H3)(3)](5) nanoclusters in the presence of TiO2 support. The gold nanoclusters exhibit good photocatalytic activity using visible light and under mild thermal conditions for the selective oxidation with molecular oxygen (O-2). The turnover frequency (TOF) of 4-methylbenzyla-mine oxidation is found to be 1522 h(-1), which is considerably higher than that conventional gold catalysts. The gold nanoclusters present good recyclability and stability for the oxidation of a wide range of amines. The superior activity of the photocatalyst is associated with its unique electronic structure and framework. The catalytically active sites are deemed to be the exposed gold atoms upon detaching protecting ligands: i.e., PPh3. The Hammett parameter suggests that the photocatalytic process involves the formation of carbocation intermediate species. Further, Au-H species were confirmed by TEMPO (2,2,6,6-tetramethylpiperidinyloxy) as a trapping agent.
关键词[WOS]: AU-25 CLUSTERS ;  AU-25(SCH2CH2PH)(18) NANOCLUSTERS ;  CO OXIDATION ;  AU CLUSTERS ;  SIZE ;  NANOPARTICLES ;  HYDROGEN ;  TIO2 ;  CATALYSIS ;  MONODISPERSE
语种: 英语
WOS记录号: WOS:000401054300066
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152304
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Gold Catalysis Res Ctr, State Key Lab Catalysis, Dalian 116023, Peoples R China
4.Carnegie Mellon Univ, Dept Chem, 4400 5th Ave, Pittsburgh, PA 15213 USA

Recommended Citation:
Chen, Haijun,Liu, Chao,Wang, Min,et al. Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines[J]. ACS CATALYSIS,2017,7:3632-3638.
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