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Preparación y estructuras moleculares y electrónicas de hierro (((0) complejos de dinitrógeno y silano y su
Suzanne C Bart1, Emil Lobkovsky, Paul J Chirik
1Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853, USA.
Journal of the American Chemical Society
|October 21, 2004
Resumen
Los nuevos complejos de dinitrógeno de hierro ((0)), (iPrPDI) Fe (((N2) 2 y (iPrPDI) Fe ((N2), son eficaces precatalizadores para la hidrogenación e hidrosilación de olefinas y alquinos. Estos catalizadores funcionan eficientemente a bajas cargas y temperaturas ambientales, ofreciendo una formación selectiva de productos anti-Markovnikov en las reacciones de hidrosilación.
Área de la Ciencia:
- Química organometálica Química orgánica de los metales.
- La catálisis de la catálisis.
Sus antecedentes:
- Los complejos de hierro son cruciales en la catálisis.
- Los ligandos de dinitrógeno pueden estabilizar los centros metálicos de baja valencia.
Objetivo del estudio:
- Para sintetizar y caracterizar nuevos complejos de hierro (((0) dinitrógeno.
- Evaluar su eficacia como precatalizadores en reacciones de hidrogenación e hidrosilación.
Principales métodos:
- Reducción de los precursores del hierro (II) con amalgama de sodio bajo atmósfera de nitrógeno.
- Caracterización espectroscópica y estructural de los complejos de hierro resultantes.
- Pruebas catalíticas para la hidrogenación e hidrosilación de sustratos insaturados.
Principales resultados:
- Síntesis de la pirámide cuadrada, de hierro de alto espín (((0) bis (((dinitrogen) complejo (iPrPDI) Fe (((N2)2) y su mono (((dinitrogen) adduct (iPrPDI) Fe (((N2).2).
- Ambos complejos demostraron una eficiente actividad precatalítica para la hidrogenación e hidrosilación de olefinas y alquinas a bajas cargas (<0,3 mol%).
- Las hidrociliaciones catalíticas produjeron selectivamente productos anti-Markovnikov; las ideas mecanicistas se obtuvieron a partir de estudios estructurales de los intermediarios y el etiquetado isotópico.
Conclusiones:
- Los nuevos complejos de hierro (((0) dinitrógeno son potentes precatalizadores para la hidrogenación y la hidrosilación.
- Los sistemas catalíticos ofrecen una alta eficiencia, selectividad y tratabilidad mecánica.
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