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Orquestación de movimientos moleculares direccionales: vías supramoleculares controladas cinéticamente de un

Xiang Wang¹, Barbara Wicher¹, Yann Ferrand¹

¹CBMN Laboratory, University of Bordeaux, CNRS, IPB, Institut Européen de Chimie Biologie, 2 rue Escarpit 33607 Pessac, France.

Journal of the American Chemical Society

|June 14, 2017

Resumen

Los investigadores diseñaron oligoamidas aromáticas de autoensamblaje para crear anfitriones de doble hélice para huéspedes oligocarbamato. Estos complejos de foldaxano demuestran movimiento molecular controlado y eventos supramoleculares complejos, que ofrecen información sobre sistemas moleculares dinámicos.

Área de la Ciencia:

Química supramolecular
Química orgánica
Ciencias de los materiales

Sus antecedentes:

Las oligoamidas aromáticas pueden autoensamblarse en estructuras complejas.
El diseño de sistemas huésped-invitado con dinámica controlable es un desafío clave en la química supramolecular.

Objetivo del estudio:

Diseñar y sintetizar un anfitrión de doble hélice capaz de enlazar huéspedes oligocarbamato lineales.
Para investigar la cinética de los hilos invitados, el deslizamiento y la disociación dentro del huésped helicoidal.
Para demostrar el potencial de los foldaxanos para la programación de eventos supramoleculares complejos.

Principales métodos:

Diseño y síntesis de huéspedes oligoamidas aromáticos y huéspedes oligocarbamatos funcionalizados.
Caracterización de la formación de complejos de foldaxano mediante resonancia magnética nuclear (RMN) y cristalografía de rayos X.
Estudios cinéticos utilizando RMN H para monitorear las dinámicas de enhebrado, deslizamiento y disociación de los huéspedes.

Principales resultados:

Formación exitosa de complejos pseudorotaxanos helicoidales (foldaxanos) entre huéspedes oligoamidas y huéspedes oligocarbamatos.
Observación de eventos cinéticos complejos durante el deslizamiento del huésped, incluida la unión intermedia y el deslizamiento rápido a lo largo de los espaciadores.
Demostración de que las barreras cinéticas pueden controlar las trayectorias supramoleculares, permitiendo la integración deliberada de los pasos de disociación-reasociación.
Se distingue entre los procesos de deslizamiento rápido (horas) y los eventos más lentos de desenrollamiento y rebobinado de la hélice (días).

Conclusiones:

Los foldaxanos proporcionan una plataforma versátil para estudiar y controlar el movimiento molecular en sistemas supramoleculares.
La cinética de los pasos individuales se puede ajustar para diseñar secuencias complejas de eventos supramoleculares.
Este trabajo avanza en los principios de diseño para arquitecturas moleculares dinámicas y materiales supramoleculares funcionales.

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