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Reactividad de los puentes de hidrógeno en grupos de espín alto [3M-3(μ-H) ] (M = FeII, CoII)
Yousoon Lee1, Kevin J Anderton1, Forrest T Sloane1
1Center for Catalysis and Department of Chemistry, University of Florida , Gainesville, Florida 32611, United States.
Journal of the American Chemical Society
|August 14, 2015
Resumen
Los nuevos grupos de hidruro metálico reaccionan selectivamente con el dióxido de carbono. La protección estérica por ligandos ciclofanos permite reacciones controladas, diferenciando la reactividad entre los complejos de hierro y cobalto para aplicaciones potenciales en catálisis.
Área de la Ciencia:
- Química organometálica
- Química de coordinación
- Ciencias de los materiales
Sus antecedentes:
- Los grupos de hidruro metálico son cruciales en la catálisis.
- Los ligandos ciclófanos ofrecen entornos estéricos únicos.
- La activación selectiva de CO2 es un desafío clave en la química.
Objetivo del estudio:
- Para sintetizar y caracterizar los nuevos grupos [3M-3(μ-H) ] (M = Fe(II), Co(II)).
- Investigar la reactividad de estos grupos con sustratos insaturados, en particular el CO2.
- Explorar la influencia de los ligandos ciclofanos en la reactividad y la selectividad de los hidritos.
Principales métodos:
- Síntesis de clústeres de Fe3H3L y Co3H3L utilizando KBEt3H.
- Difracción de rayos X monocristalino para el análisis estructural.
- Estudios de reactividad con CO2 y otras moléculas insaturadas a diferentes temperaturas.
Principales resultados:
- Los ligandos hidruro estéricamente protegidos fueron confirmados por análisis de rayos X.
- Los grupos reaccionaron selectivamente con el CO2 sobre el CS2, las alquinas y los nitriles.
- Las reacciones a temperatura ambiente produjeron mono-productos (Fe3 ((OCHO) ((H) 2L y Co3 ((OCHO) ((H) 2L), que muestran una reactividad diferencial del hidruro.
- Las reacciones de temperatura elevada revelaron una reactividad distinta: Fe3H3L formó un tri-adducto (Fe3(OCHO) 3L), mientras que Co3H3L siguió siendo un mono-adducto.
Conclusiones:
- El ligando ciclófano protege eficazmente a los ligandos hidruro, dirigiendo la reactividad selectiva del CO2.
- Se observó una reactividad diferencial de los ligandos hidruro en los grupos de hierro frente al cobalto.
- Estos hallazgos ofrecen información sobre el diseño de complejos metálicos para la captura y transformación selectiva de gases.
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