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无连接基、硅胶键合的烯烃复分解催化剂:在多相催化中的应用。

Linker-free, silica-bound olefin-metathesis catalysts: applications in heterogeneous catalysis.

机构信息

Catalysis Research Laboratory, Heidelberg, Germany.

出版信息

Chemistry. 2012 Nov 12;18(46):14717-24. doi: 10.1002/chem.201202248. Epub 2012 Sep 27.

DOI:10.1002/chem.201202248
PMID:23019012
Abstract

A set of heterogenized olefin-metathesis catalysts, which consisted of Ru complexes with the H(2)ITap ligand (1,3-bis(2',6'-dimethyl-4'dimethyl aminophenyl)-4,5-dihydroimidazol-2-ylidene) that had been adsorbed onto a silica support, has been prepared. These complexes showed strong binding to the solid support without the need for tethering groups on the complex or functionalized silica. The catalysts were tested in the ring-opening-ring-closing-metathesis (RO-RCM) of cyclooctene (COE) and the self-metathesis of methyl oleate under continuous-flow conditions. The best complexes showed a TON>4000, which surpasses the previously reported materials that were either based on the Grubbs-Hoveyda II complex on silica or on the classical heterogeneous Re(2)O(7)/B(2)O(3) catalyst.

摘要

已制备了一组由 Ru 配合物与 H(2)ITap 配体(1,3-双(2',6'-二甲基-4'-二甲基氨基苯基)-4,5-二氢咪唑-2-亚基)组成的异相烯烃复分解催化剂,该配体已被吸附到硅胶载体上。这些配合物与固体载体具有很强的结合力,而无需在配合物或官能化硅胶上使用系链基团。这些催化剂在环辛烯(COE)的开环-闭环复分解(RO-RCM)和甲基油酸的自复分解反应中在连续流动条件下进行了测试。最好的配合物表现出 TON>4000,超过了之前报道的基于硅胶上的 Grubbs-Hoveyda II 配合物或基于经典的非均相 Re(2)O(7)/B(2)O(3)催化剂的材料。

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