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Reducción catalítica selectiva de N2 a H4 por un complejo Fe simple

Peter J Hill¹, Laurence R Doyle¹, Andrew D Crawford¹

¹Department of Chemistry, Imperial College London , Imperial College Road, South Kensington, London SW7 2AZ, United Kingdom.

Journal of the American Chemical Society

|October 5, 2016

Resumen

Este estudio introduce un nuevo catalizador de hierro para la fijación selectiva de nitrógeno en hidrazina (N₂ H₄). Este avance utiliza condiciones más suaves que las informadas anteriormente para la reducción de nitrógeno molecular de hierro.

Área de la Ciencia:

Química inorgánica
Catálisis
Fijación de nitrógeno

Sus antecedentes:

La fijación catalítica del nitrógeno es crucial para la síntesis de amoníaco e hidrazina.
Pocos complejos moleculares de hierro catalizan la fijación de N2 y ninguno produce selectivamente hidrazina.
Los métodos existentes a menudo requieren reductores y ácidos duros.

Objetivo del estudio:

Desarrollar un catalizador de hierro eficiente para la fijación selectiva del nitrógeno en la hidrazina.
Investigar el uso de reductores y ácidos más suaves en la reducción de nitrógeno.
Explorar el mecanismo de formación de amoníaco en la reducción catalizada por el hierro.

Principales métodos:

Síntesis y caracterización de un complejo simple de Fe{0}, Fe{2} y PCH{2} y CH{2} y PET{2} y N{2}).
Pruebas catalíticas del complejo para la fijación de N₂ utilizando cobaltoceno (CoCp*₂) como reductor y triflato de difenilamonio (Ph₂NH₂OTf) como ácido.
Cuantificación de la producción de hidrazina (N₂ H₄) y de amoníaco (NH₃).

Principales resultados:

El complejo Fe(0) catalizó eficientemente la conversión selectiva de N₂ a N₂ H₄ (>25 volúmenes de negocio).
El amoníaco (NH₃) se produjo como un subproducto menor (aprox. 1 molécula por N₂ fijo).
Se emplearon con éxito reductores más suaves (CoCp*₂) y ácido (Ph₂NH₂OTf).

Conclusiones:

La conversión catalítica directa de N₂ al estado de oxidación de la hidrazina es viable utilizando complejos moleculares de hierro.
El sistema desarrollado demuestra una alta selectividad para la producción de N₂H₄.
El mecanismo puede involucrar intermedios Fe-N₂H₄ en la formación de NH_3.

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