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Cucurbit[8]uril y blue-box: la liberación de agua de alta energía supera las interacciones electrostáticas
Frank Biedermann1, Michele Vendruscolo, Oren A Scherman
1School of Engineering and Science, Jacobs University Bremen , Campus Ring 1, 28759 Bremen, Germany .
Journal of the American Chemical Society
|September 3, 2013
Resumen
Los investigadores desarrollaron una nueva estrategia para diseñar receptores en el agua utilizando cucurbit[8]uril (CB8) y huéspedes auxiliares (AG). La liberación de moléculas de agua confinadas impulsa la unión del analito, logrando altas afinidades de hasta 10^6 M−1.1.
Área de la Ciencia:
- Química supramolecular de las moléculas.
- Química entre anfitrión y huésped.
- Termodinámica Química es la Termodinámica Química.
Sus antecedentes:
- El diseño de receptores selectivos de analítico de alta afinidad en soluciones acuosas sigue siendo un desafío.
- Las propiedades únicas del agua influyen en los procesos de reconocimiento molecular.
- Cucurbit[8]uril (CB8) es un macrociclo rígido capaz de formar complejos con varios huéspedes.
Objetivo del estudio:
- Para presentar una nueva estrategia para el diseño de receptores en medios acuosos mediante el aprovechamiento de las propiedades del agua.
- Para investigar el mecanismo de unión de los complejos autoensamblados de cucurbita[8]urilo (CB8) y el huésped auxiliar dicationico (AG).
- Para demostrar la selectividad del analito sintonizable en estos sistemas de receptores autoensamblados.
Principales métodos:
- Simulaciones de dinámica molecular para modelar la formación compleja y el comportamiento del agua.
- Mediciones calorimétricas para determinar la termodinámica de enlace.
- Estudios sobre el efecto del disolvente y el isótopo del disolvente para apoyar el modelo de unión.
Principales resultados:
- Los complejos CB8•AG autoensamblados se unen a los analíticos liberando moléculas de agua confinadas de "alta energía".
- Esta liberación de agua proporciona una fuerza motriz entálpica significativa para la asociación.
- Se lograron constantes de unión de hasta 10^6 M−1 para los analíticos aromáticos.
- La selectividad del receptor se puede ajustar modificando el invitado auxiliar, permitiendo el reconocimiento de analytes alifáticos.
Conclusiones:
- La liberación de moléculas de agua de "alta energía" es una poderosa fuerza impulsora para la complejación huésped-huésped en solución acuosa.
- Los receptores CB8•AG autoensamblados ofrecen capacidades de reconocimiento sintonizables.
- Este enfoque ofrece una alternativa a las tradicionales interacciones anfitrión-invitado, particularmente en entornos acuosos.
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