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Issue 6, 2016
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Hydridosilylamido complexes of Ta and Mo isolobal with Berry's zirconocenes: syntheses, β-Si–H agostic interactions, catalytic hydrosilylation, and insight into mechanism

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Abstract

The syntheses of novel Group 5 and Group 6 hydrosilylamido complexes of the type R(ArN[double bond, length as m-dash])M{N(tBu)SiMe2–H}X (M = Ta, R = Cp; M = Mo, R = ArN; X = Cl, H, OBn, Me) are described. The various substituents in the X position seem to play the key role in determining the extent of β-agostic interaction with the Si–H bond. The Mo agostic hydrido complex (ArN[double bond, length as m-dash])2Mo{η3-N(tBu)SiMe2–H}H is a pre-catalyst for the hydrosilylation of carbonyls. The stoichiometric reaction between benzaldehyde and (ArN[double bond, length as m-dash])2Mo{η3-N(tBu)SiMe2–H}H gives the benzoxy complex (ArN[double bond, length as m-dash])2Mo{N(tBu)SiMe2–H}(OBn), which showed a similar catalytic reactivity compared to the parent hydride. Mechanistic studies suggest that a non-hydride mechanism is operative.

Graphical abstract: Hydridosilylamido complexes of Ta and Mo isolobal with Berry's zirconocenes: syntheses, β-Si–H agostic interactions, catalytic hydrosilylation, and insight into mechanism

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Publication details

The article was received on 19 Nov 2015, accepted on 14 Dec 2015 and first published on 18 Dec 2015


Article type: Paper
DOI: 10.1039/C5DT04548G
Dalton Trans., 2016,45, 2554-2561

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    Hydridosilylamido complexes of Ta and Mo isolobal with Berry's zirconocenes: syntheses, β-Si–H agostic interactions, catalytic hydrosilylation, and insight into mechanism

    N. A. McLeod, L. G. Kuzmina, I. Korobkov, J. A. K. Howard and G. I. Nikonov, Dalton Trans., 2016, 45, 2554
    DOI: 10.1039/C5DT04548G

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