Gott, Andrew L., Clarke, Adam J., Clarkson, Guy J. and Scott, Peter. (2007) Structure-activity relationships for group 4 biaryl amidate complexes in catalytic hydroamination/cyclization of aminoalkenes. Organometallics, Vol.26 (No.7). pp. 1729-1737. ISSN 0276-7333

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Abstract

Synthesis of bis(carboxamide) proligands derived from (R,S)-2,2'-diamino-6,6'dimethylbiphenyl was readily achieved by treatment of the amine with acid chlorides. Direct reaction with homoleptic alkyls of the group 4 metals cleanly yielded amidate complexes. These complexes were shown by single-crystal X-ray diffraction to be monomeric in the case of titanium and dimeric in the case of zirconium. The complexes formed do not yield well-defined cations upon reaction with standard borate/borane activators, and although some hydroamination catalysis was observed, it was not at a rate that is useful. In-situ treatment of Zr(NMe2)(4) with the proligands H2L1-4 yielded complexes of varying nuclearity depending on the steric bulk of the amide substituents, but in contrast to the metal alkyl series, mononuclear species are accessible; the mesityl derivative [(S)-(LZr)-Zr-4(NMe2)(2)] was found to be a highly enantioselective catalyst for the hydroamination/cyclization of 1-amino-2,2-dimethylpent-4-ene, with an enantiomeric excess of 91%.

Item Type:	Journal Article
Subjects:	Q Science > QD Chemistry
Divisions:	Faculty of Science > Chemistry
Journal or Publication Title:	Organometallics
Publisher:	American Chemical Society
ISSN:	0276-7333
Date:	26 March 2007
Volume:	Vol.26
Number:	No.7
Number of Pages:	9
Page Range:	pp. 1729-1737
Identification Number:	10.1021/om061087l
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
URI:	http://wrap.warwick.ac.uk/id/eprint/32219

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