Thiomethyl Substituted Dicopper Complexes: Attempts to Reproduce the Asymmetry of the Active Site from Type 3 Copper Enzymes

Wassim Rammal 1 Katalin Selmeczi 1, 2 Christian Philouze 1 Eric Saint-Aman 1 Jean-Louis Pierre 1 Catherine Belle 1
1 DCM - CIRE - Département de Chimie Moléculaire - Chimie Inorganique Redox Biomimétique
CNRS - Centre National de la Recherche Scientifique : UMR5250, UJF - Université Joseph Fourier - Grenoble 1, Institut de Chimie Moléculaire de Grenoble (ICMG)
Abstract : Two new dinucleating phenol-based ligands (m-HLSMe and p-HLSMe) bearing pyridine-containing pendant arms with a SMe group on one pyridine (meta or para position relative to the pyridine nitrogen atom) have been synthesized. After coordination by two copper(II) ions, the corresponding mu-phenoxido, mu-hydroxido dicopper(II) complexes were isolated and characterized by UV/Vis, EPR spectroscopy, single-crystal X-ray analysis (for the complex with the SMe substituent at the meta position) and electrochemistry. The presented compounds mimic the active site of type 3 copper enzymes and in particular the distinct environments of the copper ions. Both complexes are active as catalysts for the oxidation of 3,5-di-tert-butylcatechol to the respective quinone. The catalytic properties of the complexes depend on substrate binding, as reflected by the K-M values determined for the complexes in presence of 3,5-dtbc and are not correlated directly with the redox properties of the dicopper center.
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Journal of Inorganic and General Chemistry / Zeitschrift für anorganische und allgemeine Chemie, Wiley-VCH Verlag, 2013, 639 (8-9, SI), pp.1477-1482. 〈10.1002/zaac.201300059〉
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Soumis le : mercredi 22 mars 2017 - 16:40:16
Dernière modification le : mardi 16 janvier 2018 - 10:24:44

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Wassim Rammal, Katalin Selmeczi, Christian Philouze, Eric Saint-Aman, Jean-Louis Pierre, et al.. Thiomethyl Substituted Dicopper Complexes: Attempts to Reproduce the Asymmetry of the Active Site from Type 3 Copper Enzymes. Journal of Inorganic and General Chemistry / Zeitschrift für anorganische und allgemeine Chemie, Wiley-VCH Verlag, 2013, 639 (8-9, SI), pp.1477-1482. 〈10.1002/zaac.201300059〉. 〈hal-01494083〉

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