Solvent-dependent switch of ligand donor ability and catalytic activity of ruthenium(II) complexes containing pyridinylidene amide (PYA) n-heterocyclic carbene hybrid ligands

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Title: Solvent-dependent switch of ligand donor ability and catalytic activity of ruthenium(II) complexes containing pyridinylidene amide (PYA) n-heterocyclic carbene hybrid ligands
Authors: Leigh, Vivienne
Carleton, Daniel J.
Olguín, Juan
Müller-Bunz, Helge
Wright, L. James
Albrecht, Martin
Permanent link: http://hdl.handle.net/10197/6824
Date: 21-Jul-2014
Abstract: Chelating ligands incorporating both N-[1-alkylpyridin-4(1H)-ylidene]amide (PYA) and N-heterocyclic carbene (NHC) donor sites were prepared and used for the synthesis of ruthenium(II) complexes. Cyclic voltammetry, NMR, and UV–vis spectroscopy of the complexes indicate a solvent-dependent contribution of the limiting resonance structures associated with the ligand in solution. The neutral pyridylidene imine structure is more pronounced in apolar solvents (CH2Cl2), while the mesoionic pyridinium amide form is predominant in polar solvents (MeOH, DMSO). The distinct electronic properties of these hybrid PYA-NHC ligands in different solvents have a direct influence on the catalytic activity of the ruthenium center, e.g., in the dehydrogenation of benzyl alcohol to benzaldehyde. The activity in different solvents qualitatively correlates with the solvent permittivity.
Funding Details: European Research Council
Type of material: Journal Article
Publisher: American Chemical Society
Journal: Inorganic Chemistry
Volume: 53
Issue: 15
Start page: 8054
End page: 8060
Copyright (published version): 2014 American Chemical Society
Keywords: RedoxCatalysis
DOI: 10.1021/ic501026k
Language: en
Status of Item: Peer reviewed
Appears in Collections:Chemistry Research Collection

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