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Prueba de la hipótesis polinuclear: reducción multielectrónica de moléculas pequeñas por sitios de reacción de

Tamara M Powers¹, Theodore A Betley

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

Journal of the American Chemical Society

|July 20, 2013

Resumen

Los complejos de hierro trinuclear de alto espín activan enlaces nitrógeno-hidrógeno y nitrógeno-nitrógeno, produciendo productos de imido y nitrido. Este estudio demuestra su potencial para la activación cooperativa de moléculas pequeñas a través de sitios de reacción polinuclear.

Área de la Ciencia:

Química Inorgánica La Química Inorgánica es la química inorgánica.
Química organometálica Química orgánica de los metales.
Ciencia de los materiales Ciencia de los materiales.

Sus antecedentes:

Los complejos de hierro trinuclear de alto espín son investigados por su reactividad con sustratos a base de nitrógeno.
Comprender las propiedades electrónicas y estructurales de estos complejos es crucial para las aplicaciones catalíticas.

Objetivo del estudio:

Para explorar las capacidades de reducción de 2 y 4 electrones de un complejo de hierro trinuclear de alto espín específico, ((tbs) L) Fe3 ((thf).
Para sintetizar y caracterizar nuevos complejos de hierro imido y nitrido derivados de sustratos nitrogenados.
Investigar los efectos cooperativos de los centros de hierro polinucleares en la activación de moléculas pequeñas.

Principales métodos:

Reacciones de hidrazina, fenilhidrazina y 1,2-difenilhidrazina con ((tbs) L) Fe3 ((thf).
Síntesis y caracterización de grupos de imido y nitrido de triirón utilizando espectroscopia de Mössbauer y cristalografía de rayos X.
Estudios electroquímicos utilizando voltametría cíclica para determinar los estados de oxidación accesibles.

Principales resultados:

((tbs) L) Fe3 ((thf) facilita la reducción de la hidrazina y la fenilhidrazina para formar complejos imido ((tbs) L) Fe3 (((μ(3) -NH) y ((tbs) L) Fe3 (((μ(3) -NPh), respectivamente.
Se sintetizó y caracterizó estructuralmente el complejo de nitrido [{tbs}L) Fe3{m}{3}-N) Li{thf}3 mostrando simetría C3.
La escisión reductiva del azobenzeno produjo un complejo bis-imido ((tbs) L) Fe3((μ(3)-NPh) (((μ(2)-NPh), lo que indica una oxidación 4e(-) a una formulación (Fe(IV)) ((Fe(III)) 2.

Conclusiones:

Los complejos de hierro trinuclear de alto espín son mediadores efectivos para la reducción de sustratos NxHy a productos de imido y nitrido.
La naturaleza polinuclear de estos complejos de hierro permite la activación cooperativa de moléculas pequeñas.
Los estudios electroquímicos confirman la accesibilidad de altos estados de oxidación, hasta (Fe(IV))(Fe(III)) 2.

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