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Aceleración drástica de la transferencia selectiva de átomos de oxígeno por un complejo de hierro no hemo (IV) - oxo:

Leland R Widger¹, Casey G Davies, Tzuhsiung Yang

¹Department of Chemistry, The Johns Hopkins University , 3400 North Charles Street, Baltimore, Maryland 21218, United States.

Journal of the American Chemical Society

|January 30, 2014

Resumen

Un nuevo complejo de hierro (II) con un ligando de sulfuro permite reacciones rápidas de transferencia de átomos de oxígeno. Este estudio detalla el complejo complejo.

Área de la Ciencia:

Química bioorgánica Química bioorgánica.
Química organometálica Química orgánica de los metales.
Coordinación Química de la Coordinación

Sus antecedentes:

Los complejos de hierro son catalizadores cruciales en varias reacciones de oxidación.
Comprender el papel del entorno del ligando en la modulación de la reactividad del hierro es clave.
El desarrollo de nuevos ligandos puede desbloquear nuevas vías catalíticas.

Objetivo del estudio:

Para sintetizar y caracterizar un nuevo complejo de hierro (II) con un ligando de sulfuro.
Para investigar la reactividad del complejo de hierro en las reacciones de transferencia de átomos de oxígeno (OAT).
Para explorar la influencia de la estructura del ligando en los mecanismos OAT.

Principales métodos:

Síntesis del nuevo ligando N3Py (amida) SR y su complejo Fe (II).
Caracterización del complejo Fe (II) y su intermediario Fe (IV) oxidado.
Análisis espectroscópico y estructural para confirmar las interacciones de enlace H.
Estudios cinéticos para evaluar la actividad de OAT con varios sustratos.

Principales resultados:

Se sintetizó un nuevo complejo de Fe (II), [Fe (II) (N3Py (Amida) SR) ] (BF4) 2 (1), fue sintetizado.
Se generó una especie metastable Fe (IV) -oxo, [Fe (IV) (O) (N3Py (amida) SR) ]2+) (2), que presentaba un donante proximal de enlace H de amida.
El complejo 2 demostró una rápida OAT a sustratos de sulfuro externos.
Se logró la oxigenación directa con S, dando como resultado un complejo ligado al sulfóxido, [Fe (II) (N3Py (Amida) S (O) R) ] (BF4) 2 (4).
Se observó actividad catalítica de OAT para el complejo 1.

Conclusiones:

El nuevo ligando N3Py(amida) SR estabiliza eficazmente los estados reactivos de oxidación del hierro.
La proximidad del donante de enlace H de la amida influye en la reactividad de las especies Fe ((IV) -oxo.
El complejo de hierro exhibe potencial como catalizador para las reacciones de oxidación, particularmente la S-oxigenación.

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