On the mechanism of phenolic formylation mediated by TiCl4 complexes: existence of diradical intermediates induced by valence tautomerism

The conventional electrophilic intramolecular aromatic substitution pathway proposed by Cresp et al. [J. Chem. Soc., Perkin Trans. 1 1973, 340 345] is confirmed by the observed products of phenolic formylation mediated by TiCl4. However, when the nucleophilic path is quenched by appropriate ligand m...

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Detalles Bibliográficos
Autores: Heras, Carlos, 1986-, Ramos Tomillero, Iván, Caballero Puig, Marc, Paradís Bas, Marta, Nicolás Galindo, Ernesto, Albericio Palomera, Fernando, Moreira, Ibério de Pinho Ribeiro, Bofill i Villà, Josep M.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2015
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:2445/159605
Acceso en línea:https://hdl.handle.net/2445/159605
Access Level:acceso abierto
Palabra clave:Pèptids
Mecanismes de reacció (Química)
Radicals (Química)
Peptides
Reaction mechanisms (Chemistry)
Radicals (Chemistry)
Descripción
Sumario:The conventional electrophilic intramolecular aromatic substitution pathway proposed by Cresp et al. [J. Chem. Soc., Perkin Trans. 1 1973, 340 345] is confirmed by the observed products of phenolic formylation mediated by TiCl4. However, when the nucleophilic path is quenched by appropriate ligand modification, the initial equilibria between the possible neutral complexes of TiCl4 with 3,5-dimethoxy-phenol and/or diethyl ether lead to different stable diradical intermediates induced by valence tautomerism that provide valuable activated reagents. Some of these species have been detected by EPR, characterized theoretically and captured by TEMPO, thus providing a consistent mechanism for the reaction with one or more equivalents of TEMPO per phenol.