| Appended corrole manganese complexes:Catalysis and axial-ligand effect |
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| 作者姓名： | Nga-Chun Ng Mian HR Mahmood Chi-K.Chang Hai-Yang Liu Fei Yam Lam-Lung Yeung Chi-K.Chang |
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| 作者单位： | a Department of Chemistry and Open Laboratory of Chemical Biology of the Institute of Molecular Technology for Drug Discovery and Synthesis, Hong Kong University of Science and Technology, Hong Kong, China;
b Department of Chemistry, South China University of Technology, Guangzhou 510641, China;
c Department of Chemistry, Michigan State University, E. Lansing, MI 48824, USA |
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| 基金项目： | supported by National Natural Science Foundation of China(Nos.21171057,21371059);Research Grant Councilof Hong Kong under project HKUST6182/99p;Area of Excellence Scheme(No.AoE/P-10/01) |
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| 摘 要： | A series of N-base appended corroles and their manganese complexes were synthesized and their binding constants with three different nitrogenous ligands, triethylamine, N-methylimidazole and pyridine, were evaluated by spectroscopy. Kinetic studies indicated that the presence of appended N- donor ligands may cause a significant enhancement of the rate of oxygen atom transfers （OAT） from （oxo）manganese（V） corrole to alkene, and the stronger axial ligand binding has impact on the rate of the oxidation reaction. Turnover frequency （TOF） for the catalytic oxidation of alkenes by appended manganese corroles varies with the following ligand order： acetamido 〈 pyridyl 〈 imidazolyl. The influence of the external axial ligands on the catalytic epoxidation was investigated by using appended acetamido manganese corrole as catalyst, with the results revealing that N-methylimidazole gave the best enhancement on the yields of total oxidation products among the investigated nitrogenous ligands.
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| 关 键 词： | 锰配合物 轴向配体 催化氧化 体效应 N-甲基咪唑 环氧化反应 含氮配体 乙酰氨基 |
| 收稿时间： | 10 October 2013 |
Appended corrole manganese complexes： Catalysis and axial-ligand effect |
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| Nga-Chun Ng,Mian HR Mahmood,Chi-K.Chang,Hai-Yang Liu,Fei Yam,Lam-Lung Yeung,Chi-K.Chang.Appended corrole manganese complexes:Catalysis and axial-ligand effect[J].Chinese Chemical Letters,2014,25(4):571-574. |
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| Authors: | Nga-Chun Ng Mian HR Mahmood Hai-Yang Liu Fei Yam Lam-Lung Yeung Chi-K Chang |
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| Institution: | a Department of Chemistry and Open Laboratory of Chemical Biology of the Institute of Molecular Technology for Drug Discovery and Synthesis, Hong Kong University of Science and Technology, Hong Kong, China;
b Department of Chemistry, South China University of Technology, Guangzhou 510641, China;
c Department of Chemistry, Michigan State University, E. Lansing, MI 48824, USA |
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| Abstract: | A series of N-base appended corroles and their manganese complexes were synthesized and their binding constants with three different nitrogenous ligands,triethylamine,N-methylimidazole and pyridine,were evaluated by spectroscopy.Kinetic studies indicated that the presence of appended Ndonor ligands may cause a significant enhancement of the rate of oxygen atom transfers(OAT) from(oxo)manganese(V) corrole to alkene,and the stronger axial ligand binding has impact on the rate of the oxidation reaction.Turnover frequency(TOF) for the catalytic oxidation of alkenes by appended manganese corroles varies with the following ligand order:acetamido pyridyl imidazolyl.The influence of the external axial ligands on the catalytic epoxidation was investigated by using appended acetamido manganese corrole as catalyst,with the results revealing that N-methylimidazole gave the best enhancement on the yields of total oxidation products among the investigated nitrogenous ligands. |
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| Keywords: | Manganese Corrole Catalysis Axial-ligand Oxygen atom transfer |
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