One-Pot Synthesis of Au-11(PPh2Py)(7)Br-3 for the Highly Chemoselective Hydrogenation of Nitrobenzaldehyde
文献类型：期刊论文
| 作者 | Liu, Chao2; Abroshan, Hadi1; Yan, Chunyang2; Li, Gao2; Haruta, Masatake2 |
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2016 |
| 卷号 | 6期号:1页码:92-99 |
| 关键词 | Au Nanocluster Hydrogenation Chemoselective Dft Amine |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.5b02116 |
| 文献子类 | Article |
| 英文摘要 | In this study, the gold clusters Au-11(PPh3)(7)Cl-3 and Au-11(PPh2Py)(7)Br-3 (PPh2Py = diphenyl-2-pyridylphosphine) are synthesized via a one-pot procedure based on the wet chemical reduction method. The Au-11(PPh3)(7)Cl-3 cluster is found to be active in the chemoselective hydrogenation of 4-nitrobenzaldehyde in the presence of hydrogen (H-2) and a base (e.g., pyridine). Interestingly, the cluster with the functional ligand PPh2Py shows similar activity without losing catalytic efficiency in the absence of the base. The structure of the gold clusters and reaction pathway of the catalytic hydrogenation are investigated at the atomic/molecular level via UV vis spectroscopy, electrospray ionization (ESI) mass spectrometry, and density functional theory (DFT) calculations. It is found that one ligand (PPh3 or PPh2Py) removal is the first step to expose the core of the gold clusters to reactants, providing an active site for the catalytic reaction. Then, the H H bond of the H-2 molecule becomes activated with the aid of either free amine (base) or ligand PPh2Py which is attached to the gold clusters. This work demonstrates the promise of the functional ligand PPh2Py in the catalytic hydrogenation to reduce the amount of materials (free base: e.g., pyridine) that ultimately enter the waste stream, thereby providing a more environmentally friendly reaction medium. |
| WOS关键词 | GOLD CLUSTERS ; AU-25 CLUSTERS ; CO OXIDATION ; NANOCLUSTERS ; NANOPARTICLES ; CATALYSIS ; LIGAND ; ATOMS ; SIZE ; SEMIHYDROGENATION |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000367706800011 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/171450]  |
| 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 |
| 作者单位 | 1.Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA 2.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 | Liu, Chao,Abroshan, Hadi,Yan, Chunyang,et al. One-Pot Synthesis of Au-11(PPh2Py)(7)Br-3 for the Highly Chemoselective Hydrogenation of Nitrobenzaldehyde[J]. ACS CATALYSIS,2016,6(1):92-99. |
| APA | Liu, Chao,Abroshan, Hadi,Yan, Chunyang,Li, Gao,&Haruta, Masatake.(2016).One-Pot Synthesis of Au-11(PPh2Py)(7)Br-3 for the Highly Chemoselective Hydrogenation of Nitrobenzaldehyde.ACS CATALYSIS,6(1),92-99. |
| MLA | Liu, Chao,et al."One-Pot Synthesis of Au-11(PPh2Py)(7)Br-3 for the Highly Chemoselective Hydrogenation of Nitrobenzaldehyde".ACS CATALYSIS 6.1(2016):92-99. |
入库方式： OAI收割
来源：大连化学物理研究所
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