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Síntesis de complejos de molibdeno oxo bencilideno
Feng Zhai1, Konstantin V Bukhryakov1, Richard R Schrock1
1Department of Chemistry 6-331 , Massachusetts Institute of Technology , Cambridge , Massachusetts 02139 , United States.
Journal of the American Chemical Society
|October 9, 2018
Resumen
Este estudio detalla la síntesis y caracterización de nuevos complejos de molibdeno alquileno y bencileno. Estos compuestos de organo molibdeno exhiben una reactividad única con el agua y las olefinas, formando nuevos intermedios catalíticos.
Área de la Ciencia:
- Química organometálica
- Catálisis por molibdeno
- Química de coordinación
Sus antecedentes:
- Los complejos de molibdeno son cruciales en varias transformaciones catalíticas.
- La comprensión de la reactividad de los complejos de alquileno de molibdeno y bencilideno es clave para desarrollar nuevas metodologías sintéticas.
- Estudios anteriores han explorado sistemas relacionados, pero los patrones de reactividad específicos con ligandos voluminosos y moléculas pequeñas siguen siendo un área de interés.
Objetivo del estudio:
- Sintetizar y caracterizar nuevos complejos de molibdeno (VI) benzilideno y alquilideno con ligandos voluminosos.
- Investigar la reactividad de estos complejos con agua y olefinas.
- Para aclarar los aspectos estructurales y mecanicistas de las transformaciones observadas.
Principales métodos:
- Síntesis de complejos de molibdeno mediante reacciones con bases de amida de litio y fosfinas.
- Cristalografía de rayos X para la determinación estructural de los productos intermedios clave.
- Espectroscopia de Resonancia Magnética Nuclear (RMN) para la caracterización y el monitoreo de las reacciones.
- Reacciones con derivados de etileno y norbornadieno para estudiar la inserción de olefinas.
Principales resultados:
- Síntesis del complejo antibencilideno bipiramidal trigonal Mo(O) ((CHAro)
- Formación de complejos hidroxo-puentes diméricos tras la reacción con agua.
- Se obtienen complejos de Mo(O) ((CHArp) ((ORF9) 2 (L) con varias fosfinas.
- Sintetizó un complejo de sinalquileno de cuatro coordenadas Mo(O) ((CHArp) ((OHMT) 2.
- Se han observado reacciones con etileno que conducen a la formación de metaciclobutanos y a los intermediarios de la metátesis de olefinas.
- Se ha informado de la síntesis de productos de primera inserción con derivados del norbornadieno.
Conclusiones:
- La masa estérica del ligando OHMT influye en la geometría y la reactividad de los complejos de molibdeno.
- Los complejos de molibdeno sintetizados sirven como precursores de las especies catalíticamente relevantes.
- El estudio proporciona información sobre la reactividad fundamental de los alquildenos de molibdeno de alta valencia con sustratos insaturados.
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