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Complejos de rodio que contienen ligandos de pinza de PAlP

Naofumi Hara¹, Teruhiko Saito¹, Kazuhiko Semba¹

¹Department of Material Chemistry, Graduate School of Engineering , Kyoto University , Kyoto 615-8510 , Japan.

Journal of the American Chemical Society

|May 25, 2018

Resumen

Los nuevos complejos de rodio con ligandos de aluminilo permiten la alquilación selectiva del alqueno de la piridina. Estos catalizadores PAlP-Rh demuestran la acidez de Lewis y facilitan la alquilación de C2, lo que hace avanzar la catálisis organometálica.

Área de la Ciencia:

Química organometálica
Catálisis
Diseño del ligando

Sus antecedentes:

Los ligandos de pinza son cruciales para estabilizar los centros metálicos para aplicaciones catalíticas.
Los ligandos de aluminilo ofrecen propiedades electrónicas únicas debido al centro de aluminio.

Objetivo del estudio:

Síntesis y caracterización de nuevos complejos de rodio con ligandos de pinza PAlP con una fracción de aluminio tipo X.
Para investigar las propiedades electrónicas y la acidez de Lewis del ligando aluminílico.
Evaluar la actividad catalítica de estos complejos en la funcionalización de alquenos.

Principales métodos:

Síntesis de complejos de rodio-PAlP-aluminio.
Espectroscopia infrarroja (IR) para la caracterización electrónica.
Difracción de rayos X monocristalino para el análisis estructural.
Pruebas catalíticas para las reacciones de funcionalización C-H.

Principales resultados:

Síntesis exitosa de complejos de rodio que contienen ligandos de pinza PAlP con un grupo aluminila de tipo X.
La espectroscopia IR y la difracción de rayos X confirmaron la fuerte capacidad de donación de sigma del ligando de aluminilo.
La coordinación de la piridina con el centro de aluminio demostró la acidez de Lewis de la porción de aluminilo.
Los complejos PAlP-Rh catalizaron efectivamente la monoalquilación selectiva de C2 de la piridina con alceno.

Conclusiones:

Los nuevos complejos PAlP-Rh que contienen aluminila exhiben una acidez de Lewis significativa y fuertes propiedades de donación de sigma.
Estos complejos representan una nueva clase de catalizadores para la funcionalización selectiva C-H de las piridinas.
Los hallazgos abren vías para el desarrollo de nuevos sistemas catalíticos basados en la cooperación entre el elemento principal del grupo y los metales de transición.

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