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Unveiling the role of ancillary ligands in acceptorless benzyl alcohol dehydrogenation and etherification mediated by mesoionic carbene iridium complexes

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Abstract

We synthesized a set of triazolylidene iridium(III) complexes [IrCp*(C^N)L]n+ (Cp* = pentamethylcyclopentadienyl, C^N = C,N-bidentate coordinating pyridyl-triazolylidene) containing different neutral or anionic ancillary ligands L and evaluated their impact on the catalytic activity in alcohol conversion. We demonstrate that these ancillary ligands have a strong influence on the catalytic selectivity and direct whether the iridium center preferentially catalyzes either the dehydrogenation or the dehydration of benzyl alcohol. Ligand exchange experiments provide a direct correlation of ligand lability with catalytic activity and selectivity. These results underline the relevance of ancillary ligands and provide a rational approach to tailor the catalytic activity of the iridium center towards aldehyde formation (loss of H2) or etherification (elimination of H2O).

Graphical abstract: Unveiling the role of ancillary ligands in acceptorless benzyl alcohol dehydrogenation and etherification mediated by mesoionic carbene iridium complexes

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Publication details

The article was received on 31 Oct 2017, accepted on 26 Nov 2017 and first published on 27 Nov 2017


Article type: Paper
DOI: 10.1039/C7DT04109H
Citation: Dalton Trans., 2018, Advance Article
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    Unveiling the role of ancillary ligands in acceptorless benzyl alcohol dehydrogenation and etherification mediated by mesoionic carbene iridium complexes

    Á. Vivancos, A. Petronilho, J. Cardoso, H. Müller-Bunz and M. Albrecht, Dalton Trans., 2018, Advance Article , DOI: 10.1039/C7DT04109H

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