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Ensamblajes de huéspedes basados en resorcinareno polimétrico nanométrico que se unen fuertemente a los fullerenos
O Danny Fox1, James Cookson, Emma J S Wilkinson
1Department of Chemistry, University of Oxford, Inorganic Chemistry Laboratory, South Parks Road, Oxford, OX1 3QR, U.K.
Journal of the American Chemical Society
|May 25, 2006
Resumen
Los investigadores crearon nanoestructuras polimetales utilizando ensamblaje dirigido por metales. Estas estructuras se unen eficazmente a los fullerenos (C60 y C70) a través de las interacciones del ditoicarbamato, formando arquitecturas tipo jaula o de bucle.
Área de la Ciencia:
- Química supramolecular de las moléculas.
- Ciencia de los nanomateriales Ciencia de los nanomateriales
- Coordinación Química de la Coordinación
Sus antecedentes:
- Los cavitandos son huéspedes versátiles capaces de formar ensamblajes complejos.
- Los ligandos del dithiocarbamato ofrecen propiedades de coordinación únicas con los metales de transición.
- Los fullerenos son importantes alótropos de carbono con diversas aplicaciones.
Objetivo del estudio:
- Para sintetizar ensamblajes nanodimensionales polimetales utilizando cavitandos funcionalizados con diotiocarbamato.
- Para investigar la influencia de la geometría de coordinación del metal en las arquitecturas resultantes.
- Explorar las interacciones de unión entre estos conjuntos y los fullerenos (C60 y C70).
Principales métodos:
- Ensamblaje dirigido al metal de cavitandos funcionalizados con diotiocarbamato con metales de transición tardía (Ni, Pd, Cu, Au, Zn, Cd).
- Cristalografía de rayos X para determinar estructuras complejas (jaulas octanucleares, bucles hexanucleares).
- Métodos espectroscópicos (UV-Vis, RMN), electroquímicos, espectrometría de masas por electrospray y modelado molecular para el estudio de la unión del fullereno.
Principales resultados:
- Formación de complejos octanucleares "cagelike" con centros metálicos planos cuadrados y estructuras hexanucleares de "bucle molecular" con geometrías metálicas piramidales de base cuadrada.
- Demostración de la complementariedad estérica y electrónica entre los conjuntos anfitriones y los fullerenes.
- Fuerte unión de los fullerenos a través de los átomos de sulfuro del diotiocarbamato, con evidencia de encapsulación en complejos de cobre (II) debido a la labilidad del ligando.
Conclusiones:
- La geometría de coordinación de metales es un determinante crítico de la arquitectura de ensamblaje polimétrico.
- Las estructuras Dithiocarbamate-cavitand proporcionan sitios de unión efectivos para los fullerenos.
- La naturaleza dinámica de los enlaces metal-ditiocarbamato puede facilitar la encapsulación del huésped.
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