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Las reacciones estequiométricas y la hidrogenación catalítica con un Zr(+) / amina intramolecular reactivo frustraron
Xin Xu1, Gerald Kehr1, Constantin G Daniliuc1
1Organisch-Chemisches Institut, Universität Münster, Corrensstrasse 40, D-48149 Münster, Germany.
Journal of the American Chemical Society
|March 18, 2015
Resumen
Un nuevo catalizador de par frustrado de Lewis (FLP) basado en zirconio facilita la hidrogenación eficiente de alquenos y alquinas en condiciones suaves. Este FLP organometálico permite la escisión de dihidrógeno heterolítico y la transferencia de H ((+) / H ((-) para aplicaciones catalíticas.
Área de la Ciencia:
- Química organometálica Química orgánica de los metales.
- La catálisis es la catálisis.
- Frustrados los pares de Lewis.
Sus antecedentes:
- Los pares de Lewis frustrados (FLP) son ácidos y bases de Lewis que no pueden formar aductos clásicos, lo que lleva a una reactividad única.
- Los complejos de zirconio ofrecen potencial como nuevas plataformas de FLP debido a sus propiedades electrónicas.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo FLP basado en zirconio.
- Investigar la reactividad de este FLP con moléculas pequeñas y su potencial catalítico.
Principales métodos:
- Síntesis de un complejo de zirconio con un ligando de amina colgante.
- Activación del complejo de zirconio con un catión de tritilo para generar el FLP.
- Reacciones con diclorometano, dihidrógeno y sustratos insaturados.
Principales resultados:
- Generación de una FLP Zr(+) /amina reactiva (14) a partir de un precursor de zirconio (13).
- Demostración de la reactividad del FLP incluyendo reacciones con CH2Cl2, H2 y alquinas.
- Hidrogenación catalítica de alquenos y alquinas internas utilizando FLP 14 bajo condiciones suaves (temperatura ambiente, 1,5 bar H2).
Conclusiones:
- El FLP Zr(+) /amina (14) es un catalizador eficaz para las reacciones de hidrogenación.
- El sistema FLP exhibe una eficiente activación de dihidrógeno y capacidades de transferencia H(+) / H(-).
- Las condiciones de reacción suaves y la baja carga del catalizador (1-4 mol%) resaltan la utilidad práctica de este sistema catalítico.
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