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Observación del rebote radical en un modelo de hierro no hemo mononuclear
Thomas M Pangia1, Casey G Davies2, Joshua R Prendergast2,3
1Department of Chemistry , The Johns Hopkins University , Baltimore , Maryland 21218 , United States.
Journal of the American Chemical Society
|March 15, 2018
Resumen
Los investigadores sintetizaron un complejo de metóxido de hierro no hemo. Reacción con un clivado homolítico de enlaces hierro-oxígeno y formación de enlaces carbono-oxígeno, observando directamente el mecanismo de rebote de los radicales.
Área de la Ciencia:
- Química inorgánica
- Química bioorgánica
- Mecanismos de reacción
Sus antecedentes:
- Las enzimas de hierro no hemo juegan un papel crucial en las reacciones de oxidación biológica.
- Comprender los mecanismos de los centros de hierro no hemo es vital para diseñar imitaciones sintéticas.
- El mecanismo de rebote radical es una vía propuesta para las oxidaciones catalizadas por hierro no hemo.
Objetivo del estudio:
- Sintetizar y caracterizar un complejo de metóxido terminal de hierro no hemo.
- Investigar el mecanismo de reacción entre el complejo de hierro y un radical trifenilmetilo.
- Proporcionar evidencia experimental directa para el proceso de rebote radical en la química del hierro no hemo.
Principales métodos:
- Síntesis del complejo de metóxido de hierro no hemo [FeIII(N3PyO2Ph) ((OCH3) ]ClO4.
- Reacción del complejo de hierro con el radical trifenilmetilo (Ph3C•).
- Caracterización espectroscópica que incluye UV-vis, EPR, H NMR y espectroscopia de Mössbauer.
Principales resultados:
- Síntesis exitosa del complejo de hierro objetivo.
- Observación de la formación de Ph3 COCH3, lo que indica la formación de enlaces C-O.
- La evidencia espectroscópica confirmó la reducción del centro de hierro a hierro (II) y la escisión del enlace homolítico Fe-O.
Conclusiones:
- La reacción demuestra directamente el mecanismo de rebote radical que involucra la escisión homolítica de enlaces Fe-O y la formación de enlaces C-O.
- Este estudio proporciona información crucial sobre la reactividad de los centros de hierro no hemo.
- Los hallazgos contribuyen a la comprensión de la catálisis biológica y sintética del hierro no hemo.
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