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Hidrógenos de cobre ligados con trifosfina para la hidrogenación de CO2: estudios de estructura, reactividad y

Christopher M Zall¹, John C Linehan¹, Aaron M Appel¹

¹Pacific Northwest National Laboratory , Richland, Washington 99352, United States.

Journal of the American Chemical Society

|July 20, 2016

Resumen

Un precursor de catalizador de cobre reacciona con hidrógeno y base para formar un hidruro de cobre, que también cataliza la hidrogenación de CO2. Este hidruro de cobre puede ser un intermediario clave en el ciclo catalítico, con el hidruro de cobre mononuclear propuesto como la especie activa.

Área de la Ciencia:

Química organometálica
Catálisis
Utilización del dióxido de carbono

Sus antecedentes:

Los complejos de cobre (I) trifosfina son precursores de catalizadores activos para la hidrogenación de CO2 para formar.
La comprensión de los intermediarios catalíticos es crucial para optimizar los procesos de reducción de CO2.

Objetivo del estudio:

Investigar la reacción de un complejo de cobre (I) trifosfina con H2 y base.
Caracterizar las especies de hidruro de cobre resultantes y evaluar su actividad catalítica.
Para aclarar el mecanismo de hidrogenación de CO2 catalizado por complejos de cobre.

Principales métodos:

Síntesis y caracterización del hidruro catiónico de dicobre, [(LCu) 2H]PF6.
Determinación de la hidricidad termodinámica de [(LCu) 2 H] ((+) utilizando las constantes de equilibrio.
Reacciones estequiométricas de [(LCu) 2H] ((+) con CO2 bajo condiciones de base variables.
Análisis estructural en estado sólido de [(LCu) 2H] ((+).

Principales resultados:

El complejo de cobre ((I) LCu ((MeCN) PF6 reacciona con H2 y base para formar [ ((LCu) 2H) PF6, un precursor activo del catalizador de hidrogenación de CO2.
La hidricidad termodinámica de [(LCu) 2H] ((+) se midió en 41,0 kcal/mol.
[(LCu) 2H] ((+) reacciona estequiométricamente con CO2 para producir formato y LCu ((MeCN) ((+), con velocidades de reacción mejoradas por bases fuertes.
El hidruro de cobre mononuclear, LCuH, se propone como la especie catalíticamente activa.

Conclusiones:

El hidruro catiónico de cobre [{LCu) 2H}{+} es un intermediario relevante en la hidrogenación de CO2 catalizada por el cobre.
La actividad catalítica está significativamente influenciada por la presencia y la fuerza de coordinación de las bases.
El hidruro de cobre mononuclear LCuH se propone como el hidruro metálico activo responsable de la reducción de CO2.

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