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La captura de hidrazina y la escisión de enlaces N-N en el hierro habilitadas por ácidos de Lewis adjuntos flexibles
John J Kiernicki1, Matthias Zeller2, Nathaniel K Szymczak1
1Department of Chemistry, University of Michigan , Ann Arbor, Michigan 48109, United States.
Journal of the American Chemical Society
|December 12, 2017
Resumen
Este estudio detalla un nuevo complejo de hierro con grupos de boro que se une a la hidrazina. La reducción produce un raro complejo de hierro-diamido estabilizado por boranos, que puede liberar amoníaco.
Área de la Ciencia:
- Química organometálica
- Química del boro
- Química de coordinación
Sus antecedentes:
- Los complejos de hierro basados en pinzas son catalizadores versátiles.
- La hidrazina (N2 H4) es una fuente clave de nitrógeno en química.
- Los sitios ácidos de Lewis pueden activar moléculas pequeñas.
Objetivo del estudio:
- Síntesis y caracterización de un complejo Fe (II) a base de pinza con boranos añadidos.
- Para investigar la unión de hidrazina a este complejo.
- Explorar la reactividad de las especies resultantes, en particular la reducción y el intercambio de ligandos.
Principales métodos:
- Síntesis de un complejo Fe ((II) basado en pinzas con 9-borabiciclo [3.3.1] sustituyentes de nonilo.
- Estudios de coordinación que incluyen la unión con hidrazina (N2H4).
- Transformación reductiva del complejo Fe:N2H4.
- Experimentos de protonación y intercambio de ligandos.
Principales resultados:
- El complejo Fe (II) exhibe acidez de Lewis, lo que permite la unión de 1-2 equivalentes de hidrazina.
- La reducción del 1:1 Fe:N2H4 adducto forma un único complejo Fe (NH) 2.
- Los ligandos de amido en el complejo Fe (NH) se estabilizan por interacciones con los grupos de boro.
- El amoníaco (NH3) puede ser liberado durante la protonación, lo que permite el intercambio exógeno de hidrazina.
Conclusiones:
- Los complejos Fe ((II) a base de pinzas con boranos adjuntos pueden activar y estabilizar los derivados de hidrazina.
- El sistema desarrollado ofrece una vía a especies raras de diamido de hierro.
- El sistema demuestra potencial para la liberación y el intercambio controlados de ligandos que contienen nitrógeno.
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