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La transferencia del grupo oxidativo a un complejo de triirón para formar un nucleófilo μ(3)-nitruro, [Fe3(μ(3)-N) ]-
Tamara M Powers1, Alison R Fout, Shao-Liang Zheng
1Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street, Cambridge, Massachusetts 02138, United States.
Journal of the American Chemical Society
|February 22, 2011
Resumen
Los investigadores sintetizaron un nuevo complejo trinuclear de hierro que reacciona con azida para formar un complejo de nitruro. Este nitruro puede ser metilado, creando un complejo de metilimida, mostrando un enlace único hierro-nitrógeno.
Área de la Ciencia:
- Coordinación Química de la Coordinación
- Química organometálica Química orgánica de los metales.
- Síntesis Inorgánica y Síntesis Inorgánica.
Sus antecedentes:
- Los complejos trinucleares de hierro son de interés por sus propiedades magnéticas y catalíticas únicas.
- Comprender la reactividad de las especies de nitruro metálico e imida es crucial para la investigación de la fijación del nitrógeno.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo complejo de hierro trinuclear ligado a hexadentato.
- Para investigar la reactividad de este complejo con azida inorgánica.
- Para explorar la subsiguiente alquilación del complejo de nitruro resultante.
Principales métodos:
- Síntesis de un ligando hexadentado y su correspondiente complejo trinuclear de hierro.
- Caracterización mediante técnicas espectroscópicas y cristalográficas.
- Reacción del complejo de hierro con azido de tetrabutylamonio seguido de metilación con yoduro de metilo.
Principales resultados:
- Síntesis exitosa de un complejo de hierro trinuclear de alto espín, ((tbs) L) Fe ((3)).
- Formación de un complejo de nitruro trinuclear aniónico, [{tbs) L) Fe{3}{micro{3}-N}NBu{4}, tras la reacción con azida.
- Conversión del nitruro en un complejo de metilimida neutro, ((tbs) L) Fe ((3) (((micro ((3) -NCH ((3)), a través de la metilación.
Conclusiones:
- El ligando hexadentado facilita la formación de un núcleo de hierro trinuclear asimétrico.
- El complejo trinuclear de nitruro de hierro exhibe un ligando de nitruro piramidalizado y enlaces cortos Fe-Fe.
- El ligando de nitruro puede ser fácilmente alquilado para formar una metilimida, manteniendo la integridad estructural del complejo.
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