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Issue 5, 2013
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Rare earth metal bis(silylamide) complexes bearing pyridyl-functionalized indenyl ligand: Synthesis, structure and performance in the living polymerization of L-lactide and rac-lactide

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Abstract

Amine elimination of rare earth tris(silylamide) complexes Ln[N(SiHMe2)2]3(THF)2 (Ln = La, Sm, Er, Lu) with 1 equiv. of the pyridyl-functionalized indenyl ligand C9H7CMe2CH2C5H4N-α afforded a series of neutral mono-indenyl-ligated rare earth metal bis(silylamide) complexes (C9H6CMe2CH2C5H4N-α)Ln[N(SiHMe2)2]2 (Ln = La (1), Sm (2), Er (3), Lu (4)) in 83–87% isolated yields. Reaction of La[N(SiHMe2)2]3(THF)2 with 2 equivalents of C9H7CMe2CH2C5H4N-α provided the neutral bis(indenyl) lanthanum mono(silylamide) complex (C9H6CMe2CH2C5H4N-α)2LaN(SiHMe2)2 (5). These complexes were characterized by elemental analysis, FT-IR and NMR (except for 3 for the strong paramagnetic property of the central metal). X-ray single crystal structural diffraction showed that 1–4 are isostructural and the central metals are four-coordinated by one indenyl ring, one nitrogen atom from the pendant pyridyl group, and two amide groups to form a distorted tetrahedral geometry; while the central metal in 5 is five-coordinated by two indenyl rings, two nitrogen atoms from the pendant pyridyl groups, and one amide group to adopt a distorted pyramidal geometry, if the indenyl ring is regarded as occupying an independent vertex. The monoanionic pyridyl-functionalized indenyl ligand is bonded to the central metal in η51 constrained geometry configuration (CGC) mode. 1–4 are highly active for the ring-opening polymerization of L-lactide and rac-lactide. In the presence of 2 equivalents of benzyl alcohol, 1 shows high activity toward L-lactide and rac-lactide in a living fashion.

Graphical abstract: Rare earth metal bis(silylamide) complexes bearing pyridyl-functionalized indenyl ligand: Synthesis, structure and performance in the living polymerization of l-lactide and rac-lactide

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Publication details

The article was received on 10 Sep 2012, accepted on 06 Nov 2012 and first published on 12 Nov 2012


Article type: Paper
DOI: 10.1039/C2DT32083E
Citation: Dalton Trans., 2013,42, 1862-1871
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    Rare earth metal bis(silylamide) complexes bearing pyridyl-functionalized indenyl ligand: Synthesis, structure and performance in the living polymerization of L-lactide and rac-lactide

    Y. Wang, Y. Lei, S. Chi and Y. Luo, Dalton Trans., 2013, 42, 1862
    DOI: 10.1039/C2DT32083E

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