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Caracterización de las especies de hierro-imido relevantes para la química de transferencia del grupo N

Diana A Iovan¹, Theodore A Betley¹

¹Department of Chemistry and Chemical Biology, Harvard University , 12 Oxford Street, Cambridge, Massachusetts 02138, United States.

Journal of the American Chemical Society

|January 21, 2016

Resumen

Este estudio sintetizó un nuevo complejo de hierro que reacciona con azidas de arilo para formar especies de imido terminales o puentes. Estos complejos de imido de hierro muestran potencial como catalizadores para las reacciones de transferencia de grupos N y la aminación C-H.

Área de la Ciencia:

Química organometálica
Química de coordinación
Catálisis

Sus antecedentes:

Los complejos de hierro son cruciales en varias transformaciones catalíticas.
Comprender la reactividad de las especies de imido de hierro es clave para desarrollar nuevos sistemas catalíticos.
Los ligandos estérilmente obstaculizados pueden influir en la estabilidad y la reactividad de los complejos metálicos.

Objetivo del estudio:

Síntesis y caracterización de nuevos complejos de di-hierro-dipirrinato sustituidos por tert-butilo.
Investigar la reactividad de estos complejos con las azidas de arilo, formando especies de imido de hierro.
Explorar el potencial catalítico de los complejos de imido de hierro resultantes en las reacciones de transferencia de grupos N y de aminación C-H.

Principales métodos:

Síntesis de un complejo de di-hierro-dipirrinato sustituido por tert-butilo.
Reacción con varios azidos de arilo para formar complejos de imido de hierro terminal y puente.
(57) Espectroscopia de Mössbauer y cristalografía de rayos X para la caracterización estructural y electrónica.
Magnetometría SQUID y magnetometría de estado sólido para determinar las propiedades magnéticas.
Monitoreo in situ para observar los intermedios catalíticos.

Principales resultados:

Síntesis exitosa de un complejo de di-hierro de dipirrinato sustituido por tert-butilo estéricamente accesible.
Formación de dos imidos de hierro distintos: un imido de hierro terminal y un di-hierro puente, dependiendo de la estructura de azido de arilo.
Caracterización de las estructuras electrónicas y propiedades magnéticas de las especies de imido de hierro, incluidos los centros Fe ((III) de alto espín.
Demostración de la di-ferro imido puente como un reactivo de transferencia de grupo N competente y una especie catalíticamente activa en la aminación C-H.

Conclusiones:

El complejo de hierro sintetizado proporciona acceso a diversas especies de imido de hierro con reactividad ajustable.
El complejo di-hierro imido puente exhibe actividad catalítica en las reacciones de transferencia de HAA y N-grupo.
Estos hallazgos destacan el potencial de los complejos de imido de hierro como catalizadores versátiles en la síntesis orgánica.

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