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Issue 24, 2016
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Modification of silica-supported tungsten neosilyl oxo precatalysts: impact of substituted phenol on activity and stability in olefin metathesis

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Abstract

A novel strategy to access a large variety of tungsten oxo pre-catalysts for olefin metathesis involving post-treatment of [([triple bond, length as m-dash]SiO)W([double bond, length as m-dash]O)(CH2SiMe3)3], 1b, with the desired spectator ligands is presented. This method allowed establishing structure–reactivity relationships in propylene metathesis as a function of the spectator ligands of tungsten oxo species. Thus, the novel pre-catalysts [([triple bond, length as m-dash]SiO)W([double bond, length as m-dash]O)R2X], 2a–c (X = 2,6-dimethylphenoxide, 2-trifluoromethylphenoxide, pentafluorophenoxide), are obtained by modification of well-defined monopodal species 1b by substituted phenols along with TMS release. These were demonstrated by mass balance analysis, elemental analysis, IR, advanced solid-state NMR (1D and 2D 1H, 13C and 19F) and EXAFS. The modified materials were proved to lead to stable and efficient supported tungsten oxo catalysts for propene metathesis under dynamic conditions at 80 °C.

Graphical abstract: Modification of silica-supported tungsten neosilyl oxo precatalysts: impact of substituted phenol on activity and stability in olefin metathesis

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Publication details

The article was received on 24 Aug 2016, accepted on 05 Nov 2016 and first published on 08 Nov 2016


Article type: Paper
DOI: 10.1039/C6CY01812B
Citation: Catal. Sci. Technol., 2016,6, 8532-8539
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    Modification of silica-supported tungsten neosilyl oxo precatalysts: impact of substituted phenol on activity and stability in olefin metathesis

    Y. Bouhoute, I. Del Rosal, K. C. Szeto, N. Merle, D. Grekov, A. De Mallmann, E. Le Roux, L. Delevoye, R. M. Gauvin, L. Maron and M. Taoufik, Catal. Sci. Technol., 2016, 6, 8532
    DOI: 10.1039/C6CY01812B

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