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[Fe₄] y [Fe₆] Agrupaciones de hidrógenos apoyadas por fosfinas: síntesis, caracterización y aplicación en la

Ryoichi Araake, Kazuki Sakadani, Mizuki Tada

¹Department of Chemistry, Daido University , Takiharu-cho, Minami-ku, Nagoya 457-8530, Japan.

Journal of the American Chemical Society

|April 4, 2017

Resumen

Los nuevos grupos de hidrógeno de hierro catalizan la sililación del nitrógeno (N₂). Estos grupos de hierro convierten eficientemente el N2 en productos sililados en condiciones suaves, ofreciendo una vía potencial para la fijación de nitrógeno.

Área de la Ciencia:

Química inorgánica
Química organometálica
Catálisis

Sus antecedentes:

Múltiples átomos de hierro conectados por hidritos son motivos estructurales clave en la reducción de nitrógeno (N₂).
La comprensión del papel de estas especies de hidrógeno de hierro es crucial tanto para la fijación biológica como industrial de N2.

Objetivo del estudio:

Para sintetizar y caracterizar nuevos grupos de hierro soportados por hidruro.
Investigar la actividad catalítica de estos grupos de hierro en la sililación N2.

Principales métodos:

Reacción de un complejo de Fe (II) amida con pinacolborano en presencia o ausencia de fosfinas.
Caracterización cristalográfica y espectroscópica de los cúmulos resultantes [Fe₄] y [Fe₆].
Pruebas catalíticas de los racimos sintetizados para la silificación de N₂ en condiciones ambientales.

Principales resultados:

Síntesis de grupos de hierro bien definidos soportados por hidrógeno: Fe₄(μ-H)₄(μ₃-H)₂{N(SiMe₃)₂}₂(PR₃)₄ y Fe₆(μ-H)₁₀(μ₃-H)₂(P₃)₁₀.
La silición catalítica de N2 por estos racimos produjo hasta 160 ± 13 equivalentes de N3 por racimo de Fe4 y 183 ± 18 equivalentes por racimo de Fe6.
La espectrometría de masas y la formación de adutos sugirieron la disociación de ligandos (fosfina e hidruro) como parte del ciclo catalítico.

Conclusiones:

Los grupos de hierro soportados por hidrógeno son catalizadores efectivos para la sililación de N2.
La actividad catalítica es significativa y se ha observado un alto volumen de ventas.
La disociación de ligandos juega un papel en la generación de especies catalíticas activas.

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