Isomerization of a cationic (η5-C5Me5)Ir(III) complex involving remote C–C and C–H bond formation

The reactivity of an unsaturated, cationic (C5Me5)Ir(III) complex (2(Xyl)þ) bearing the xylyl-substituted terphenyl phosphine PMe2ArXyl2 (ArXyl2 = C6H3-2,6-(C6H3-2,6-Me2)2) towards triethylamine (NEt3) is studied and compared to our previous investigations based on the related complex 2(Dipp)þ conta...

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Detalles Bibliográficos
Autores: Moreno, Juan J., Espada, María F., Maya, Celia, Campos, Jesús, López-Serrano, Joaquín, Macgregor, Stuart A., Carmona, Ernesto
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2021
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/247571
Acceso en línea:http://hdl.handle.net/10261/247571
Access Level:acceso abierto
Palabra clave:Iridium
DFT
Terphenyl phosphine
Organometallic
C5Me5
Descripción
Sumario:The reactivity of an unsaturated, cationic (C5Me5)Ir(III) complex (2(Xyl)þ) bearing the xylyl-substituted terphenyl phosphine PMe2ArXyl2 (ArXyl2 = C6H3-2,6-(C6H3-2,6-Me2)2) towards triethylamine (NEt3) is studied and compared to our previous investigations based on the related complex 2(Dipp)þ containing the bulkier phosphine PMe2ArDipp2 (ArDipp2 = C6H3-2,6-(C6H3-2,6-iPr2)2). Low-temperature multinuclear NMR studies support the formation of a C–C bond between the deprotonated C5Me5 ligand and a flanking xylyl ring of the phosphine, which becomes dearomatized (complex 4(Xyl)þ). Interestingly, this complex presents divergent reactivity relative to the bulkier diisopropylphenyl counterpart, undergoing formal addition of HCl to yield complex 5 (Xyl)þ, isomeric to the starting complex 2(Xyl)þ. These transformations are rationalized by means of Density Functional Theory (DFT) calculations