Item


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. © 2014 The Royal Society of Chemistry

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

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
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. © 2014 The Royal Society of Chemistry
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
Document access: http://hdl.handle.net/2072/296989
Language: eng
Publisher: Royal Society of Chemistry (RSC)
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: Recercat

Subjects

Authors


Warning: Unknown: write failed: No space left on device (28) in Unknown on line 0

Warning: Unknown: Failed to write session data (files). Please verify that the current setting of session.save_path is correct (/var/lib/php5) in Unknown on line 0