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Reducción catalítica de N2 a NH3 por un complejo Fe-N2 con un anclaje de átomo C

Sidney E Creutz¹, Jonas C Peters

¹Division of Chemistry and Chemical Engineering, California Institute of Technology , Pasadena, California 91125, United States.

Journal of the American Chemical Society

|December 20, 2013

Resumen

Los investigadores exploraron el papel de un átomo de carbono central en el cofactor de hierro-molibdeno (FeMoco) utilizando la química del modelo de hierro-dinitrógeno (Fe-N2). Descubrieron que este átomo de carbono puede unirse al dinitrógeno, lo que permite una modesta conversión catalítica de N2 a amoníaco.

Área de la Ciencia:

Química bioorgánica Química bioorgánica.
Química organometálica Química orgánica de los metales.
La catálisis de la catálisis.

Sus antecedentes:

El cofactor de hierro-molibdeno (FeMoco) en la MoFe-nitrogenasa contiene un átomo de carbono intersticial central, cuya función sigue sin estar clara.
Estudios previos sugieren que este átomo de carbono puede desempeñar un papel en la unión y activación del sustrato.

Objetivo del estudio:

Investigar el papel de un donante de carbono axial en los complejos de hierro para la unión y reactividad del dinitrógeno.
Para explorar la hipótesis de que el carbono intersticial en FeMoco facilita la unión del dinitrógeno a través de una interacción trans.

Principales métodos:

Síntesis y caracterización estructural de nuevos complejos de hierro con un ligando tris (((fosfino) alquilo con un donante de carbono axial.
Análisis espectroscópico y cristalográfico de complejos de hierro-dinitrógeno en múltiples estados de oxidación.
Evaluación de la actividad catalítica de un complejo aniónico hierro-dinitrógeno para la síntesis de amoníaco.

Principales resultados:

Se sintetizaron complejos de hierro con el ligando alquilo tris (((phosphino), que se unen al trans-nitrógeno dinitrógeno al donante de carbono axial.
El análisis estructural reveló el alargamiento del enlace Fe-C ((alquilo) tras la reducción, lo que indica un carácter iónico.
El complejo aniónico, (CP ((iPr) 3) FeN2 ((-), fue funcionalizado con un electrofilo sililo y demostró una actividad catalítica modesta para la reducción de N2 a NH3.

Conclusiones:

El donante de carbono axial en el sistema modelo se une efectivamente al dinitrógeno, apoyando su papel potencial en FeMoco.
El comportamiento de enlace Fe-C ((alquilo) observado sugiere una interacción flexible crucial para la función de la nitrogenasa.
El complejo de hierro desarrollado sirve como un modesto catalizador para la fijación de nitrógeno, ofreciendo información sobre el mecanismo de la nitrogenasa.

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