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Issue 5, 2012
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Oxygen extrusion from amidate ligands to generate terminal Ta[double bond, length as m-dash]O units under reducing conditions. How to successfully use amidate ligands in dinitrogen coordination chemistry

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Abstract

A series of mixed Cp* amidate tantalum complexes Cp*Ta(RNC(O)R′)X3 (where R = Me2C6H3, iPr, R′ = tBu, Ph, X = Cl, Me) have been prepared via salt metathesis and their fundamental reactivities under reducing conditions have been explored. Reaction of the tantalum chloro precursors with potassium graphite under N2 or Ar leads to the stereoselective formation of the terminal tantalum oxo species, Cp*Ta[double bond, length as m-dash]O(η2-RN[double bond, length as m-dash]CR′)Cl. This represents the formal extrusion of oxygen from the amidate ligand to the reduced tantalum center and is accompanied by the formation of the iminoacyl fragment bound to Ta(V). Amidate dinitrogen complexes, [Cp*TaCl(RNC(O)tBu)]2(μ-N2) (where R = Me2C6H3, iPr) were synthesized via salt metathesis from the known [Cp*TaCl2]2(μ-N2) precursor, establishing that amidate ligands can support dinitrogen complexes, but not the reduction process often necessary for their synthesis.

Graphical abstract: Oxygen extrusion from amidate ligands to generate terminal Ta [[double bond, length as m-dash]] O units under reducing conditions. How to successfully use amidate ligands in dinitrogen coordination chemistry

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Publication details

The article was received on 24 Aug 2011, accepted on 24 Oct 2011 and first published on 07 Dec 2011


Article type: Paper
DOI: 10.1039/C1DT11595B
Citation: Dalton Trans., 2012,41, 1609-1616

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    Oxygen extrusion from amidate ligands to generate terminal Ta[double bond, length as m-dash]O units under reducing conditions. How to successfully use amidate ligands in dinitrogen coordination chemistry

    P. Horrillo-Martinez, B. O. Patrick, L. L. Schafer and M. D. Fryzuk, Dalton Trans., 2012, 41, 1609
    DOI: 10.1039/C1DT11595B

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