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Construcción selectiva de muy grandes nodos metálicos inducidos por interacción de apilamiento y anillo borromeo

Hai-Ning Zhang¹, Yue-Jian Lin¹, Guo-Xin Jin^1,2

¹Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, Department of Chemistry, Fudan University, Shanghai 200433, P.R. China.

Journal of the American Chemical Society

|December 31, 2020

Resumen

Los investigadores sintetizaron nodos metálicos moleculares complejos y anillos borromeos utilizando ligandos específicos. El cambio del ligando alteró el resultado a los metalociclos, destacando el papel de las interacciones de apilamiento en el ensamblaje molecular.

Área de la Ciencia:

Química de coordinación
Química supramolecular
Ciencias de los materiales

Sus antecedentes:

Las arquitecturas moleculares complejas son cruciales para el desarrollo de materiales avanzados.
Comprender las fuerzas intermoleculares es clave para controlar los procesos de autoensamblaje.
Las estructuras orgánicas metálicas y los polímeros de coordinación ofrecen diversas posibilidades estructurales.

Objetivo del estudio:

Para sintetizar nuevos nudos de metal molecular y anillos borromeos.
Investigar el papel de la estructura del ligando y las interacciones intermoleculares en el autoensamblaje.
Explorar la formación de diferentes estructuras supramoleculares mediante la modificación de los ligandos.

Principales métodos:

Reacciones multicomponentes que utilizan ligandos dipirídicos y iones metálicos específicos (rodio).
Cristalografía de rayos X para una aclaración estructural detallada de los conjuntos resultantes.
Variación sistemática del volumen del ligando para observar cambios en los resultados de autoensamblaje.

Principales resultados:

Síntesis de alto rendimiento de dos nodos metálicos moleculares (más de 500 átomos no hidrógenos, 16 iones Rh) y un anillo borromeo.
Confirmación estructural a través de la cristalografía de rayos X.
La sustitución del ligando inicial por un análogo más voluminoso dio lugar a la formación de tres metalociclos tetranucleares, lo que demuestra la sensibilidad a los efectos estéricos.

Conclusiones:

Las interacciones intermoleculares, particularmente el apilamiento pi-pi, son críticas para la formación de nudos metálicos y anillos de Borromeo.
El diseño de ligandos influye significativamente en la arquitectura supramolecular resultante.
El obstáculo estérico introducido por la modificación del ligando puede redirigir las vías de autoensamblaje hacia diferentes estructuras como los metalociclos.

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