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Polypyrrole-functionalized ruthenium carbene catalysts as efficient heterogeneous systems for olefin epoxidation

New Ru complexes containing the bpea-pyr ligand (bpea-pyr stands for N,N-bis(pyridin-2-ylmethyl)-3-(1H-pyrrol-1-yl)propan-1-amine), with the formula [RuCl2(bpea-pyr)(dmso)] (isomeric complexes 2a and 2b) or [Ru(CN-Me)(bpea-pyr)X)]n+ (CN-Me = 3-methyl-1-(pyridin-2-yl)-1H- imidazol-3-ium-2-ide; X = Cl, 3, or X = H2O, 4), have been prepared and fully characterized. Complexes 3 and 4 have been anchored onto an electrode surface through electropolymerization of the attached pyrrole group, yielding stable polypyrrole films. The electrochemical behaviour of 4, which displays a bielectronic Ru(IV/II) redox pair in solution, is dramatically affected by the electropolymerization process leading to the occurrence of two monoelectronic Ru(IV/III) and Ru(III/II) redox pairs in the heterogeneous system. A carbon felt modified electrode containing complex 4 (C-felt/poly-4) has been evaluated as a heterogeneous catalyst in the epoxidation of various olefin substrates using PhI(OAc)2 as an oxidant, displaying TON values of several thousands in all cases and good selectivity for the epoxide product

This research was financed by MINECO of Spain through projects CTQ2010-21532-C02-01, CTQ2012-32436 and CTQ2009-08328. The authors acknowledge STR from UdG for technical support

© Dalton Transactions, 2014, vol. 43, núm. 26, p. 9916-9923

Royal Society of Chemistry (RSC)

Manager: Ministerio de Ciencia e Innovación (Espanya)
Author: Dakkach, Mohamed
Fontrodona, Xavier
Parella Coll, Teodor
Atlamsani, Ahmed
Romero García, Isabel
Rodríguez Pizarro, Montserrat
Date: 2014
Abstract: New Ru complexes containing the bpea-pyr ligand (bpea-pyr stands for N,N-bis(pyridin-2-ylmethyl)-3-(1H-pyrrol-1-yl)propan-1-amine), with the formula [RuCl2(bpea-pyr)(dmso)] (isomeric complexes 2a and 2b) or [Ru(CN-Me)(bpea-pyr)X)]n+ (CN-Me = 3-methyl-1-(pyridin-2-yl)-1H- imidazol-3-ium-2-ide; X = Cl, 3, or X = H2O, 4), have been prepared and fully characterized. Complexes 3 and 4 have been anchored onto an electrode surface through electropolymerization of the attached pyrrole group, yielding stable polypyrrole films. The electrochemical behaviour of 4, which displays a bielectronic Ru(IV/II) redox pair in solution, is dramatically affected by the electropolymerization process leading to the occurrence of two monoelectronic Ru(IV/III) and Ru(III/II) redox pairs in the heterogeneous system. A carbon felt modified electrode containing complex 4 (C-felt/poly-4) has been evaluated as a heterogeneous catalyst in the epoxidation of various olefin substrates using PhI(OAc)2 as an oxidant, displaying TON values of several thousands in all cases and good selectivity for the epoxide product
This research was financed by MINECO of Spain through projects CTQ2010-21532-C02-01, CTQ2012-32436 and CTQ2009-08328. The authors acknowledge STR from UdG for technical support
Format: application/pdf
Citation: 023159
ISSN: 1477-9226 (versió paper)
1477-9234 (versió electrònica)
Document access: http://hdl.handle.net/10256/11713
Language: eng
Publisher: Royal Society of Chemistry (RSC)
Collection: MICINN/PN 2011-2014/CTQ2010-21532-C02-01
Reproducció digital del document publicat a: http://dx.doi.org/10.1039/c4dt00698d
Articles publicats (D-Q)
Is part of: © Dalton Transactions, 2014, vol. 43, núm. 26, p. 9916-9923
Rights: Tots els drets reservats
Subject: Catalitzadors
Catalysts
Catàlisi heterogènia
Heterogeneous catalysis
Title: Polypyrrole-functionalized ruthenium carbene catalysts as efficient heterogeneous systems for olefin epoxidation
Type: info:eu-repo/semantics/article
Repository: DUGiDocs

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