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首页> 外文期刊>Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology >Supramolecular assembly of chiral polyoxometalate complexes for asymmetric catalytic oxidation of thioethers
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Supramolecular assembly of chiral polyoxometalate complexes for asymmetric catalytic oxidation of thioethers

机译：手性多金属氧酸盐配合物的超分子组装，用于硫醚的不对称催化氧化

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In this paper, a chiral amphiphilic cation with two stereocenters has been employed to encapsulate a well-known catalytically activated sandwich-type polyoxometalate, Na_(12)[WZn3(H2O)2(ZnW9O_(34))2], through electrostatic interaction. The prepared chiral organic cation-encapsulated polyoxometalate complexes were found to self-aggregate into spherical supramolecular assemblies with a diameter of ca. 100 nm in the reaction solution. These assemblies, serving as microreactors, exhibited an efficient asymmetric catalytic activity for the oxidation of sulfide with up to 72% enantiomeric excess. The coverage density of chiral organic cations enwrapped on the polyoxometalate surface was proved to have an important influence on the enantioselectivity. Detailed kinetic study of the catalytic process showed that the enantioselectivity of sulfide oxidation was derived from the combination of an ineffective asymmetric sulfoxidation and an effective kinetic resolution of the sulfoxide. The present research strategically offers an understanding for the direct and efficient construction of polyoxometalate based supramolecular catalysts for asymmetric reactions through controlling the surface microenvironment.
机译：在本文中，具有两个立构中心的手性两亲阳离子已被用于通过静电相互作用封装众所周知的催化活化的夹心型多金属氧酸盐Na_（12）[WZn3（H2O）2（ZnW9O_（34））2]。发现所制备的手性有机阳离子包封的多金属氧酸盐配合物能自聚集成直径约3μm的球形超分子组装体。在反应溶液中为100 nm。这些用作微反应器的组件对硫化物的氧化表现出有效的不对称催化活性，对映体过量高达72％。事实证明，包裹在多金属氧酸盐表面上的手性有机阳离子的覆盖密度对对映选择性具有重要影响。催化过程的详细动力学研究表明，硫化物的对映选择性是无效亚砜的不对称不对称氧化和有效动力学拆分的综合结果。本研究从战略上为通过控制表面微环境直接有效地构建基于多金属氧酸盐的不对称反应的超分子催化剂提供了一种理解。

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