The first group 4 metal bis(imido) and tris(imido) complexes

Andrew D. Schwarz; Alastair J. Nielson; Nikolas Kaltsoyannis; Philip Mountford

doi:10.1039/C1SC00786F

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Chemical Science

Issue 3, 2012

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The first group 4 metal bis(imido) and tris(imido) complexes

Andrew D. Schwarz,^a Alastair J. Nielson,*^b Nikolas Kaltsoyannis*^c and Philip Mountford*^a

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Chemistry Research Laboratory, University of Oxford, Mansfield Road, Oxford, UK
E-mail: philip.mountford@chem.ox.ac.uk.

Department of Chemistry, Institute of Natural Sciences, Massey University at Auckland, Private Bag 102 904, North Shore Mail Centre, Auckland, New Zealand
E-mail: A.J.Nielson@massey.ac.nz.

Department of Chemistry, University College London, Christopher Ingold Laboratories, 20 Gordon Street, London, UK
E-mail: n.kaltsoyannis@ucl.ac.uk.

Chem. Sci., 2012,3, 819-824

DOI: 10.1039/C1SC00786F
Received 11 Oct 2011, Accepted 09 Nov 2011
First published online 09 Nov 2011

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We report a combined experimental and computational study of the first bis(imido) and tris(imido) complexes of a group 4 metal. Reaction of [Ti(NAr)(NHAr)₂(py)₂] (1, Ar = 2,6-C₆H₃ⁱPr₂) with 3 equivs. of MeLi gave the lithium-stabilised tris(imide) [TiMe(NAr)₃{Li(py)}₃] (2). Reaction of 1 with 2 equivs. of MeLi in the presence of ArNH₂ gave the corresponding bis(imide) [Ti(NAr)₂(NHAr)₂{Li(py)}₂] (3). All three compounds 1, 2 and 3 have substantial Ti–N_imide multiple bond character. Orbital and Mayer bond order analysis show that the formal bond orders are best viewed as ca. 3, 2.5 and 2, respectively, with a further attenuating effect on the multiple bonding by the [Li(py)]⁺ ion coordination. Compounds 2 and 3 are the first examples of any group 4 metal simultaneously containing two or three multiply-bonded ligands.

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