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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes
Published on: April 10, 2015
¿Puede favorecerse la desproporción del estado de oxidación III en los sistemas RuII-OH2/RuIV=O?
Ester Masllorens1, Montserrat Rodríguez, Isabel Romero
1Departament de Química, Universitat de Girona, Campus de Montilivi, E-17071 Girona, Spain.
Journal of the American Chemical Society
|April 20, 2006
Resumen
Se sintetizaron y caracterizaron tres nuevos complejos rutenio-agua. Estos complejos exhiben propiedades electroquímicas únicas y reactividad estereoselectiva en reacciones de oxidación, con aplicaciones potenciales en catálisis.
Área de la Ciencia:
- Coordinación Química de la Coordinación
- Química organometálica Química orgánica de los metales.
- La catálisis de la catálisis.
Sus antecedentes:
- Los complejos rutenio-agua son importantes en la catálisis y en la química redox.
- Los entornos de los ligandos de afinación tienen un impacto significativo en las propiedades complejas de los metales.
Objetivo del estudio:
- Para sintetizar y caracterizar nuevos complejos rutenio-agua con carbenos mezclados y ligandos pirídicos.
- Para investigar el comportamiento electroquímico y la reactividad catalítica de estos nuevos complejos.
Principales métodos:
- Síntesis y caracterización estructural (difracción de rayos X, RMN).
- Estudios electroquímicos (voltametría cíclica, voltametría de pulso diferencial, coulombimetría).
- Oxidación catalítica del cis-beta-metilestireno.
Principales resultados:
- Se prepararon y caracterizaron con éxito tres nuevos complejos Ru-aqua, [Ru ((CNC) ((bpy) ((H2O) ] ((PF6) 2 (1) y cis-/trans- [Ru ((CNC) ((nBu-CN) ((H2O) ] ((PF6) 2 (cis-2 y trans-2).
- El complejo 1 mostró una mínima diferencia de potencial redox (DeltaE1/2) de 50 mV a pH 7.
- Los complejos cis-2 y trans-2 mostraron estados de oxidación inestables de Ru(III) y una epoxidación altamente estereoselectiva del cis-beta-metilestireno, produciendo sólo cis-epoxido.
Conclusiones:
- Los complejos Ru-aqua sintetizados poseen distintas propiedades electroquímicas influenciadas por su entorno de ligando.
- Existe una fuerte correlación inversa entre DeltaE1/2 y la estereoselectividad en las reacciones de epoxidación.
- Estos hallazgos ponen de relieve el potencial de los complejos Ru-aqua adaptados en la catálisis estereoselectiva.
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