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Cobalto bien definido ((I) catalizador de dihidrógeno: evidencia experimental para un proceso de redox Co ((I) / Co

Kenan Tokmic¹, Charles R Markus¹, Lingyang Zhu¹

¹School of Chemical Sciences, University of Illinois at Urbana-Champaign , 600 South Mathews Avenue, Urbana, Illinois 61801, United States.

Journal of the American Chemical Society

|August 30, 2016

Resumen

Un nuevo complejo de dihidrógeno de cobalto, sintetizado a partir de un precursor de cobalto (I) -dinitrógeno, cataliza eficientemente la hidrogenación de alquenos a temperatura ambiente. Este complejo facilita el intercambio hidrógeno-deuterio y participa en un ciclo redox de cobalto (I) / cobalto (III).

Área de la Ciencia:

Química organometálica
Catálisis
Síntesis inorgánica

Sus antecedentes:

Los complejos de cobalto son cruciales en la catálisis.
Los ligandos de pinza ofrecen propiedades electrónicas y estéricas únicas.
La comprensión de los ciclos redox es clave para el diseño del catalizador.

Objetivo del estudio:

Para sintetizar y caracterizar un complejo de dihidrógeno de cobalto.
Para investigar su actividad catalítica en la hidrogenación de alquenos.
Para aclarar el mecanismo utilizando técnicas avanzadas de RMN.

Principales métodos:

Síntesis de un complejo precursor de cobalto (I) -dinitrógeno.
Preparación de un complejo de dihidrógeno de cobalto utilizando un ligando de pinza bis ((carbeno).
Caracterización espectroscópica que incluye transferencia de RMN por polarización multinuclear y inducida por parahidrógeno (PHIP).
Hidrogenación catalítica de alquenos a temperatura ambiente.

Principales resultados:

Síntesis exitosa de un complejo de dihidrógeno de cobalto Co (I) - (H2).
Se ha demostrado la mezcla H2/D2 y la hidrogenación de alquenos a temperatura ambiente.
Caracterización de un intermediario de clorhidrato de Co (III).
Regeneración del precursor de CO2 a través de la evolución del hidrógeno.

Conclusiones:

El complejo de cobalto sintetizado es un catalizador activo para la hidrogenación de alquenos.
Las especies Co ((I) - ((H2) juegan un papel vital en el ciclo redox catalítico.
Los estudios avanzados de RMN proporcionan información mecanicista sobre el proceso catalítico.

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