Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines
Chen, Haijun2,3; Liu, Chao4; Wang, Min2; Zhang, Chaofeng2; Luo, Nengchao2,3; Wang, Yehong2; Abroshan, Hadi1; Li, Gao4; Wang, Feng2
刊名ACS CATALYSIS
2017-05-01
卷号7页码:3632-3638
关键词Gold Nanoclusters Au-25 Photocatalysis Selective Organic Transformation Benzylamine Oxidation
DOI10.1021/acscatal.6b03509
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.
语种英语
WOS记录号WOS:000401054300066
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/152304]  
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
作者单位1.Carnegie Mellon Univ, Dept Chem, 4400 5th Ave, Pittsburgh, PA 15213 USA
2.Chinese Acad Sci, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, Gold Catalysis Res Ctr, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式
GB/T 7714
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.
APA Chen, Haijun.,Liu, Chao.,Wang, Min.,Zhang, Chaofeng.,Luo, Nengchao.,...&Wang, Feng.(2017).Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines.ACS CATALYSIS,7,3632-3638.
MLA Chen, Haijun,et al."Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines".ACS CATALYSIS 7(2017):3632-3638.
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