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Acoplamiento mediado por hierro de dióxido de carbono y etileno: las metallactonas macrocíclicas permiten el acceso a
Stephan M Rummelt1, Hongyu Zhong1, Ilia Korobkov2
1Department of Chemistry , Princeton University , Princeton , New Jersey 08544 , United States.
Journal of the American Chemical Society
|September 4, 2018
Resumen
Los complejos de hierro reaccionan con dióxido de carbono y etileno para formar productos carboxilados. Los intermediarios de metalactona son clave para generar carboxilatos de hierro saturados y insaturados a través de las inserciones de etileno.
Área de la Ciencia:
- Química organometálica
- Química de coordinación
- Catálisis
Sus antecedentes:
- Los complejos de hierro con ligandos de diimina voluminosos (PDI) son catalizadores versátiles.
- Los ligandos de nitrógeno en los complejos de hierro pueden ser fácilmente desplazados por otros sustratos.
Objetivo del estudio:
- Investigar la reactividad de un complejo hierro-nitrógeno con dióxido de carbono y etileno.
- Elucidar el mecanismo de formación de los productos de carboxilato de hierro.
Principales métodos:
- Reacción de (iPrPDI) Fe ((N2) 2) con el CO2 y el etileno.
- Caracterización estructural de los productos de carboxilato de hierro mediante cristalografía de rayos X.
- Estudios de etiquetado de deuterio para sondear las vías de reacción.
Principales resultados:
- Formación de una serie homóloga de productos de carboxilato de hierro saturados y insaturados.
- Identificación de un intermediario de metalactona de cinco miembros.
- La inserción de etileno en la metallactona da lugar a productos macrocíclicos.
Conclusiones:
- La reacción se lleva a cabo a través de intermediarios de metallactona, seguidos de inserciones de etileno.
- La distribución del producto está controlada por las proporciones de reactivo.
- Los complejos de hierro pueden facilitar la escisión de enlaces C-O y la formación de enlaces C-C.
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