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Influence of ligand backbone flexibility in group 4 metal complexes of tetradentate mixed tertiary amine/alkoxide ligands

Influence of ligand backbone flexibility in group 4 metal complexes of tetradentate mixed tertiary amine/alkoxide ligands
Influence of ligand backbone flexibility in group 4 metal complexes of tetradentate mixed tertiary amine/alkoxide ligands
Simple epoxide ring opening chemistry using the cyclic secondary amine 1,4-diazacycloheptane or the related linear species N,N'-dimethylethylenediamine, and racemic (+/-) -3,3-dimethyl-1,2-epoxybutane gives access to the pendant alcohol functionalised ditertiary amine pro-ligands [HOCH(Bu-t)CH2N(R)CH2](2) (H2L1:R-2=CH2CH2CH2; H2L2:R-2=Me-2). The contrasting reactions of H2L1 and H2L2 towards homoleptic group 4 alkoxides highlight the crucial role of ligand backbone flexibility in complex formation. Thus, the chemistry of the more conformationally rigid system (L-1)(2-) appears to be constrained by the cyclic ligand core, such that it adopts a bridging (mu(2):eta(2), eta(2)) mode of coordination towards Ti(IV), leading to dinuclear metal systems [e.g. (LTi2)-Ti-1((OPr)-Pr-i)(6)]. By contrast, the more flexible linear system (L-2)(2-) binds to both Ti(IV) and Zr(IV) in a chelating fashion leading, for example, to the synthesis of the C-2 symmetric mononuclear complex rac-(LTi)-Ti-2((OPr)-Pr-i)(2). Thus, a simple synthesis of diastereomerically pure, C-2 symmetric, geometrically cis octahedral Ti(IV) complexes from racemic precursors is presented.
olefin polymerization catalysts, arm triazacyclononane ligands, schiff-base complexes, extra donor arm, titanium complexes, zirconium complexes, bis(phenolato) ligand, living polymerization, ethylene polymerization, 1-hexene polymerization
1144-0546
135-142
Day, Joanna K.
46d4e919-f0ad-4b85-8c88-ea5be867c605
Baghurst, Rebecca E.
9921beae-e8b2-46dc-b445-6467d869f23f
Strevens, Robert R.
bf0a5347-4cec-44cd-b3b5-48b6f782a4d8
Light, Mark E.
cf57314e-6856-491b-a8d2-2dffc452e161
Hursthouse, Michael B.
57a2ddf9-b1b3-4f38-bfe9-ef2f526388da
Stengel, Bruno F.
e85b0c97-5800-4235-bf4f-b59bf432bdeb
Fallis, Ian A.
6f14a47a-a4f7-405d-94eb-33fe818a21c5
Aldridge, Simon
de66448a-0f63-4b8b-ac55-f78dcd4830ea
Day, Joanna K.
46d4e919-f0ad-4b85-8c88-ea5be867c605
Baghurst, Rebecca E.
9921beae-e8b2-46dc-b445-6467d869f23f
Strevens, Robert R.
bf0a5347-4cec-44cd-b3b5-48b6f782a4d8
Light, Mark E.
cf57314e-6856-491b-a8d2-2dffc452e161
Hursthouse, Michael B.
57a2ddf9-b1b3-4f38-bfe9-ef2f526388da
Stengel, Bruno F.
e85b0c97-5800-4235-bf4f-b59bf432bdeb
Fallis, Ian A.
6f14a47a-a4f7-405d-94eb-33fe818a21c5
Aldridge, Simon
de66448a-0f63-4b8b-ac55-f78dcd4830ea

Day, Joanna K., Baghurst, Rebecca E., Strevens, Robert R., Light, Mark E., Hursthouse, Michael B., Stengel, Bruno F., Fallis, Ian A. and Aldridge, Simon (2007) Influence of ligand backbone flexibility in group 4 metal complexes of tetradentate mixed tertiary amine/alkoxide ligands. New Journal of Chemistry, 31 (1), 135-142. (doi:10.1039/b608680b).

Record type: Article

Abstract

Simple epoxide ring opening chemistry using the cyclic secondary amine 1,4-diazacycloheptane or the related linear species N,N'-dimethylethylenediamine, and racemic (+/-) -3,3-dimethyl-1,2-epoxybutane gives access to the pendant alcohol functionalised ditertiary amine pro-ligands [HOCH(Bu-t)CH2N(R)CH2](2) (H2L1:R-2=CH2CH2CH2; H2L2:R-2=Me-2). The contrasting reactions of H2L1 and H2L2 towards homoleptic group 4 alkoxides highlight the crucial role of ligand backbone flexibility in complex formation. Thus, the chemistry of the more conformationally rigid system (L-1)(2-) appears to be constrained by the cyclic ligand core, such that it adopts a bridging (mu(2):eta(2), eta(2)) mode of coordination towards Ti(IV), leading to dinuclear metal systems [e.g. (LTi2)-Ti-1((OPr)-Pr-i)(6)]. By contrast, the more flexible linear system (L-2)(2-) binds to both Ti(IV) and Zr(IV) in a chelating fashion leading, for example, to the synthesis of the C-2 symmetric mononuclear complex rac-(LTi)-Ti-2((OPr)-Pr-i)(2). Thus, a simple synthesis of diastereomerically pure, C-2 symmetric, geometrically cis octahedral Ti(IV) complexes from racemic precursors is presented.

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Published date: 2007
Keywords: olefin polymerization catalysts, arm triazacyclononane ligands, schiff-base complexes, extra donor arm, titanium complexes, zirconium complexes, bis(phenolato) ligand, living polymerization, ethylene polymerization, 1-hexene polymerization

Identifiers

Local EPrints ID: 44578
URI: http://eprints.soton.ac.uk/id/eprint/44578
ISSN: 1144-0546
PURE UUID: ae061bf1-a7fb-4777-b6b1-96c5a5ac82c0
ORCID for Mark E. Light: ORCID iD orcid.org/0000-0002-0585-0843

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Date deposited: 02 Mar 2007
Last modified: 16 Mar 2024 03:04

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Contributors

Author: Joanna K. Day
Author: Rebecca E. Baghurst
Author: Robert R. Strevens
Author: Mark E. Light ORCID iD
Author: Bruno F. Stengel
Author: Ian A. Fallis
Author: Simon Aldridge

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