Selective oxidation of alcohols with hydrogen peroxide catalyzed by hexadentate binding 8-quinolinolato manganese(III) complexes
Selective oxidation of alcohols with hydrogen peroxide catalyzed by hexadentate binding 8-quinolinolato manganese(III) complexes
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六齿结合 8-羟基喹啉锰 (III) 络合物催化过氧化氢选择性氧化醇
DOI：
10.1016/j.jcat.2008.11.011
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发表时间：
2009
影响因子：
7.3
通讯作者：
Zhou, Xiaoping
中科院分区：
文献类型：
--
作者：
Ye, Zhengpei;Liu, Fenglan;Zhong, Sheng;Yin, Dulin;Fu, Zaihui;Xie, Fang;Zhou, Xiaoping
合成了一系列8-羟基喹啉锰（III）六齿配合物，通过元素分析、固体紫外-可见光谱和Hartree-Fock/3- 21 G+计算，证明其具有畸变的八面体构型.这些Mn（III）配合物被发现比它们相应的四齿8-喹啉锰（II）和salen-MnIIIOAc更有效地用于在丙酮介质中氧化醇，这是由于它们特殊的六齿结合结构，可以在过氧化氢水溶液的存在下打开轴向MnO键以形成更活跃的五齿结构，如由UV-vis光谱所支持的。配体芳环上的卤素取代基可以显著提高催化活性，其中5-氯-7-碘-8-喹啉锰（III）的转化数（TON）最高。提出了该催化体系的反应机理。
A series of hexadentate 8-quinolinolato manganese(III) complexes were synthesized and proven to own a distorted octahedral geometry via elemental analysis, solid UV–vis spectroscopy and Hartree–Fock/3-21G+ calculation. These Mn(III) complexes were found to be more efficient than their corresponding tetradentate 8-quinolinolato manganese(II) and salen-MnIIIOAc for the oxidation of alcohols in acetone medium, being due to their special hexadentate binding structures that could open an axial MnO bond to form the more active pentadentate structures in the presence of aqueous hydrogen peroxide, as supported by UV–vis spectra. The halogen substituents in ligand's aryl ring could significantly enhance the catalytic activities and 5-chloro-7-iodo-8-quinolinolato manganese(III) gave the highest turnover number (TON). A reasonable mechanism for the present catalytic system was proposed.
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