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...

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Detalles Bibliográficos
Autores: Dakkach, Mohamed, Fontrodona, Xavier, Parella Coll, Teodor, Atlamsani, Ahmed, Romero García, Isabel, Rodríguez Pizarro, Montserrat
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2014
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/11713
Acceso en línea:http://hdl.handle.net/10256/11713
Access Level:acceso embargado
Palabra clave:Catalitzadors
Catalysts
Catàlisi heterogènia
Heterogeneous catalysis
Descripción
Sumario: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