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Síntesis de la plantilla de Vernier de los nudos moleculares
Zoe Ashbridge1, Elisabeth Kreidt1, Lucian Pirvu1
1Department of Chemistry, University of Manchester, Oxford Road, Manchester M13 9PL, UK.
Science (New York, N.Y.)
|March 3, 2022
Resumen
La síntesis de nudos moleculares complejos ahora es más eficiente utilizando ligandos y iones metálicos coordinadamente incompatibles con la plantilla de Vernier. Este método permite la creación de nudos moleculares más grandes y estructurados con precisión, incluidas arquitecturas intrincadas de triskelion.
Área de la Ciencia:
- Química supramolecular
- Síntesis orgánica
- Química de coordinación
Sus antecedentes:
- Los métodos tradicionales para sintetizar nudos moleculares a menudo se basan en helicatos metálicos.
- Lograr nudos moleculares más grandes y complejos ha sido un desafío significativo en la química supramolecular.
Objetivo del estudio:
- Desarrollar una estrategia más efectiva para sintetizar nudos moleculares más grandes.
- Explorar el uso de la plantilla de Vernier con componentes que no coinciden coordinadamente.
Principales métodos:
- Se utilizan ligandos oligodentados y iones metálicos de desajuste coordinado para la plantilla de Vernier.
- Se emplean hebras de tridentato 2,6-piridindicarboxamida que se pliegan alrededor de nueve iones lantánidos de coordenadas ((III).
- Se ha completado la formación de nudos mediante metástasis de olefinas de cierre de anillo.
Principales resultados:
- Un ensamblaje Vernier de 3:2 (filamento ditópico: metal) produjo con éxito nudos de abuela +31 # +31 y -31 # -31 .
- Una estequiometría 3:4 (filamento tetratópico: metal) formó selectivamente un nudo triskelion de trébol de trébols de 378 átomos con 12 cruces de filamento alternados.
- Al alterar la estereoquímica de las hebras, se sintetizó un nudo triskelion de núcleo invertido con cruces mixtos alternados y no alternados.
Conclusiones:
- Los ligandos y los iones metálicos que no coinciden coordinadamente ofrecen un enfoque superior para sintetizar nudos moleculares más grandes a través de la plantilla de Vernier.
- Esta metodología permite un control preciso de la topología y la complejidad de los nudos, incluida la formación de nudos polinodados intrincados.
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