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La activación catalítica de CO2 asistida por hidruro de renio/B(C6F5)3 frustró los pares de Lewis -hidruros metálicos
Yanfeng Jiang1, Olivier Blacque, Thomas Fox
1Anorganisch-chemisches Institut, Universität Zürich, Winterthurerstraß 190, CH-8037 Zürich, Switzerland.
Journal of the American Chemical Society
|April 27, 2013
Resumen
Este estudio presenta un nuevo sistema de pares de Lewis frustrados (FLP) para la activación y reducción cooperativa de CO2. Los catalizadores a base de renio demuestran una hidrogenación catalítica eficiente del CO2 para formar, destacando la importancia de la masa estérica de la base y la basicidad.
Área de la Ciencia:
- Química organometálica Química orgánica de los metales.
- La catálisis es la catálisis.
- Química verde es la química verde.
Sus antecedentes:
- Los pares de Lewis frustrados (FLP) son cruciales para la activación de moléculas pequeñas.
- Los complejos de renio ofrecen una reactividad única para las transformaciones catalíticas.
- La utilización de CO2 sigue siendo un desafío importante en la química sostenible.
Objetivo del estudio:
- Desarrollar un nuevo sistema FLP para la activación y reducción cooperativa de CO2.
- Para investigar la hidrogenación catalítica de CO2 para formar el uso de catalizadores basados en renio.
- Para aclarar el papel de los ácidos y bases de Lewis en la hidrogenación de CO2.
Principales métodos:
- Síntesis y caracterización de complejos renio-borilo.
- Espectroscopia de Resonancia Magnética Nuclear (RMN) y cálculos de la Teoría Funcional de la Densidad (DFT).
- Estudios catalíticos para la hidrogenación de CO2 utilizando varias bases.
Principales resultados:
- Formación de una especie estable de tipo FLP [ReHBr ((NO) ((PR3) 2 (((η2) -OCO-B ((C6F5) 3) ] que permita la activación cooperativa del CO2.
- Generación de complejos renio-borilo y un complejo formato dihidrógeno.
- Hidrogenación catalítica exitosa de CO2 para formar con frecuencias de rotación de hasta 9 h-1.1.
- Identificación de la masa estérica y la basicidad de la base como factores críticos para una catálisis eficiente.
Conclusiones:
- El sistema de FLP de borilo-renio desarrollado activa y reduce efectivamente el CO2.
- La hidrogenación catalítica del CO2 para formar se logra con una alta eficiencia.
- El estudio proporciona información sobre el mecanismo de hidrogenación de CO2 y el papel de la selección de la base.
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