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Selección ortogonal y fijación de vías de autoensamblaje de coordinación para la construcción de conjuntos
Michael J Burke1, Gary S Nichol1, Paul J Lusby1
1EaStCHEM School of Chemistry, University of Edinburgh , Joseph Black Building, David Brewster Road, Edinburgh, Scotland EH9 3FJ, U.K.
Journal of the American Chemical Society
|June 29, 2016
Resumen
Este estudio introduce una nueva estrategia de "ensamblaje seguido de fijación" para la química supramolecular. Este método logra estructuras robustas con altos rendimientos, superando las limitaciones del control termodinámico tradicional en el autoensamblaje.
Área de la Ciencia:
- Química supramolecular
- Ciencias de los materiales
- Síntesis Química
Sus antecedentes:
- El ensamblaje supramolecular tradicional se basa en el control termodinámico, que a menudo requiere una compensación entre la reversibilidad y la estabilidad estructural.
- Los métodos existentes pueden limitar la robustez cinética de las estructuras autoensambladas.
Objetivo del estudio:
- Presentar una estrategia alternativa de "ensamblaje seguido de fijación" para una construcción supramolecular robusta.
- Para demostrar la síntesis de helicatos M2L3 y tetraedros M4L6 cinéticamente robustos.
- Para explorar el cambio de respuesta a estímulos entre diferentes arquitecturas supramoleculares.
Principales métodos:
- Utilizando el enfoque de "ensamblaje seguido de fijación" en condiciones no ambientales para atrapar cinéticamente las estructuras deseadas.
- Utilizando ligandos bis (bidentados) para la construcción de helicatos M2L3 y tetraedros M4L6.
- Investigación de estímulos redox y de luz para inducir el cambio estructural entre arquitecturas.
Principales resultados:
- Logró una síntesis de alto rendimiento y eficiencia atómica de conjuntos supramoleculares con robustez cinética similar a la covalente.
- Se ha demostrado la formación selectiva de helicatos M2L3 termodinámicamente desfavorecidos mediante la congelación del proceso de ensamblaje.
- Mostró un cambio exitoso inducido por estímulos (redox, luz) entre arquitecturas tetraédricas y helicadas.
Conclusiones:
- La estrategia de "ensamblaje seguido de fijación" ofrece una poderosa alternativa al control termodinámico en la química supramolecular.
- Este enfoque permite la creación de estructuras cinéticamente robustas y permite un control preciso sobre los resultados del ensamblaje.
- Potencial demostrado para materiales supramoleculares dinámicos y sensibles a través de transformaciones arquitectónicas inducidas por estímulos.
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