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Robustas estructuras orgánicas metálicas basadas en corróleo con clusters raros de Zr/Hf-Oxo conectados de 9 puntos
Yanming Zhao1,2,3, Shibo Qi4, Zheng Niu2
1School of Chemical Engineering and Technology , Tianjin University , Tianjin 300350 , People's Republic of China.
Journal of the American Chemical Society
|August 22, 2019
Resumen
Informamos de las primeras estructuras metal-orgánicas (MOF) basadas en corroles, Corrole-MOF-1 y Corrole-MOF-2, que ofrecen estructuras robustas y alta estabilidad. El Corrole-MOF-1 que contiene hierro demuestra una catálisis heterogénea eficiente para las reacciones de Diels-Alder.
Área de la Ciencia:
- Coordinación Química de la Coordinación
- Ciencia de los materiales Ciencia de los materiales.
- La catálisis es la catálisis.
Sus antecedentes:
- Los coroles son ligandos importantes en la química de coordinación, ofreciendo propiedades electrónicas únicas para los cationes metálicos.
- A pesar de su promesa, las unidades de corrol están subrepresentadas en materiales cristalinos porosos para la funcionalidad avanzada.
- Faltan estudios sistemáticos que integren los corroles en materiales porosos funcionales.
Objetivo del estudio:
- Para construir nuevos marcos metálico-orgánicos (MOF) basados en corroles.
- Investigar la estabilidad y la actividad catalítica de estos nuevos MOFs.
- Explorar su potencial en catálisis heterogénea, específicamente para las reacciones de Diels-Alder.
Principales métodos:
- Síntesis de dos robustos MOFs basados en corroles utilizando un ligando tricarboxilato corrolico C2-simétrico personalizado y racimos Zr6/Hf6 D3-simétricos.
- Caracterización de los MOFs, revelando una rara estructura de red gfy conectada (3,9) conectada.
- Preparación de un MOF de corrol de hierro catiónico (Corrole-MOF-1(Fe)) para estudios catalíticos.
Principales resultados:
- Construcción exitosa de Corrole-MOF-1 (Zr) y Corrole-MOF-2 (Hf) con alta estabilidad química en un amplio rango de pH.
- Los MOFs exhiben una rara topología gfy conectada (3,9).
- Corrole-MOF-1(Fe) demostró una catálisis heterogénea eficiente para las reacciones [4 + 2] hetero-Diels-Alder, superando a los catalizadores de MOF homogéneos y porfirínicos.
Conclusiones:
- Los MOFs basados en corrol desarrollados representan un avance significativo en el diseño de materiales porosos.
- Estos MOF ofrecen una excelente estabilidad y características estructurales únicas.
- El corrole-MOF-1 ((Fe) muestra un potencial prometedor como un catalizador heterogéneo altamente efectivo para transformaciones orgánicas específicas.
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