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Efectos del disolvente sobre la unión del huésped y la dinámica de una jaula Fe(II) 4L4
Jeanne L Bolliger1, Tanya K Ronson, Masahiro Ogawa
1Department of Chemistry, University of Cambridge , Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Journal of the American Chemical Society
|September 17, 2014
Resumen
Este estudio presenta una jaula de coordinación de hierro flexible que adapta su tamaño y preferencia de unión en función del disolvente. Puede encapsular moléculas grandes, incluso aquellas con conformaciones desfavorables, demostrando una química sintonizable entre huésped y huésped.
Área de la Ciencia:
- Química supramolecular de las moléculas.
- Coordinación Química de la Coordinación
- Química entre anfitrión y huésped.
Sus antecedentes:
- Las jaulas de coordinación autoensambladas ofrecen entornos únicos para el reconocimiento molecular.
- El control de las interacciones anfitrión-invitado en la solución sigue siendo un desafío.
- Las jaulas adaptativas pueden superar las limitaciones de las estructuras rígidas del huésped.
Objetivo del estudio:
- Desarrollar una jaula de coordinación sensible al disolvente para la química sintonizable entre huésped y huésped.
- Investigar la encapsulación de diversas moléculas invitadas, incluidas aquellas con conformaciones desfavorables.
- Para explorar la capacidad de la jaula para inducir cambios conformacionales en los huéspedes.
Principales métodos:
- Síntesis y caracterización de una jaula de coordinación Fe(II) 4L4 autoensamblada.
- Estudios de solubilidad en agua y acetonitrilo basados en pruebas comparativas.
- Estudios de unión cuantitativa utilizando varios huéspedes aromáticos y alifáticos.
- Espectroscopia de Resonancia Magnética Nuclear (RMN) de temperatura variable para estudiar la flexibilidad de la jaula.
Principales resultados:
- La jaula Fe(II) 4L4 exhibe solubilidad dependiente del disolvente y selectividad del huésped (agua vs. acetonitrilo).
- Tanto los huéspedes aromáticos como los alifáticos se unen en el agua, mientras que solo los alifáticos se unen en el acetonitrilo.
- Los bloques de construcción flexibles de la jaula le permiten expandirse / contraerse, acomodando a huéspedes pequeños y grandes.
- Los huéspedes grandes encapsulados adoptan conformaciones no favorecidas termodinámicamente.
- El interior quiral de la jaula puede diferenciar las señales de protones invitados.
Conclusiones:
- Una jaula de coordinación Fe(II) 4L4 adaptativa demuestra una química anfitrión-invitado sintonizable influenciada por el disolvente.
- La flexibilidad de la jaula permite un fuerte control de unión y conformación sobre los huéspedes.
- Este sistema ofrece nuevas posibilidades para el diseño de materiales supramoleculares sensibles.
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