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Un caténano de 5 pliegues simétricos entrelazados
Tanya K Ronson1, Yujia Wang2, Kim Baldridge2
1Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Journal of the American Chemical Society
|May 27, 2020
Resumen
Los investigadores crearon nuevas jaulas moleculares entrelazadas y catenanas utilizando derivados de coranuleno. Estas estructuras complejas, con iones metálicos y ligandos de piridina o fenantrolina, exhiben arreglos únicos de cuenco en cuenco con huéspedes.
Área de la Ciencia:
- Química supramolecular
- Química de coordinación
- Ciencias de los materiales
Sus antecedentes:
- Los derivados del coranuleno sirven como bloques de construcción versátiles en la química supramolecular.
- La síntesis de arquitecturas complejas entrelazadas como catenas y jaulas es un desafío significativo.
- Las jaulas metálico-orgánicas y las catenanas ofrecen aplicaciones potenciales en la química huésped-huésped y la catálisis.
Objetivo del estudio:
- Síntesis y caracterización de nuevas estructuras supramoleculares derivadas de un precursor de pentakis ((4-aminotiofenil) corannuleno.
- Investigar la formación de cadenas entrelazadas [2] y de jaulas metal-orgánicas.
- Explorar las propiedades anfitrión-invitado y las contribuciones energéticas dentro de estos conjuntos.
Principales métodos:
- Síntesis asistida por plantilla que incluye sim-pentakis ((4-aminothiophenyl) corannulene con ligandos específicos de piridina y fenantrolina y iones metálicos (CuI, CoII, ZnII).
- Caracterización estructural mediante cristalografía de rayos X, espectroscopia de resonancia magnética nuclear (RMN) y espectrometría de masas.
- Análisis computacional utilizando la Teoría Funcional de Densidad (DFT) para evaluar las contribuciones energéticas.
Principales resultados:
- Síntesis exitosa de S10-simétrico, 5 veces entrelazado [2]catenanes ([CuI5L2]5+) y D5-simétrico metal-orgánico jaulas ([MII5L2]10+).
- La cristalografía de rayos X confirmó las intrincadas estructuras de jaula y catenas interpenetradas.
- Los cálculos de DFT revelaron que las fuerzas dispersivas no covalentes juegan un papel crucial, comparable a las energías de enlace covalente.
Conclusiones:
- El estudio demuestra la viabilidad de construir arquitecturas supramoleculares complejas y multicomponentes con alta simetría.
- Las reacciones de intercambio de subcomponentes indican una preferencia por la formación de jaulas sobre la formación de catenanos en condiciones específicas.
- Las jaulas y catenanas resultantes pueden encapsular huéspedes de corannulene, formando subestructuras de tazón en tazón únicas.
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