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Microfluidic On-chip Capture-cycloaddition Reaction to Reversibly Immobilize Small Molecules or Multi-component Structures for Biosensor Applications

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Captura y liberación reversible de un ligando mediado por un interruptor de polaridad de largo alcance en un

Steven M Wales¹, David T J Morris¹, Jonathan Clayden¹

¹School of Chemistry, University of Bristol, Bristol BS8 1TS, U.K.

Journal of the American Chemical Society

|February 10, 2022

Resumen

Los investigadores sintetizaron nuevas oligoureas con enlaces de hidrógeno intercambiables. Estos foldamers dinámicos pueden controlar de forma remota la unión de ligandos, lo que demuestra una nueva forma de transmitir información molecular para sistemas químicos avanzados.

Área de la Ciencia:

Química supramolecular
Química de los polímeros
Síntesis orgánica

Sus antecedentes:

El enlace de hidrógeno juega un papel crucial en el reconocimiento molecular y el autoensamblaje.
El diseño de moléculas sintéticas con propiedades de unión controlables es esencial para materiales y sistemas químicos avanzados.

Objetivo del estudio:

Sintetizar y caracterizar las oligoureas con puente de etileno con una red de enlaces de hidrógeno conmutables.
Investigar la influencia de la ubicación del sitio de unión en la afinidad del ligando.
Para demostrar el control remoto sobre la unión del ligando a través de estímulos externos.

Principales métodos:

Síntesis de oligoureas con puentes de etileno con sitios de unión específicos.
Análisis espectroscópico para confirmar la estructura y el enlace de hidrógeno.
Estudios de unión de ligandos para evaluar la afinidad y la cinética de liberación.
Experimentos controlados por pH para inducir y revertir cambios conformacionales.

Principales resultados:

Se sintetizaron con éxito oligoureas con una cadena de enlaces de hidrógeno continua y conmutable.
La afinidad de unión de los ligandos dependía de la posición del sitio de unión (donante vs. receptor).
Desprotonación/reprotonación remota de un grupo ácido terminal modulado por la polaridad del enlace de hidrógeno y la unión del ligando.
La liberación y la recaptura de ligandos se lograron a través de un cambio conformacional remoto transmitido a través de la cadena de oligourea.

Conclusiones:

Este estudio presenta el primer sistema molecular sintético capaz de transmitir información de unión intermolecular.
Las estructuras plegables dinámicas ofrecen una plataforma novedosa para el desarrollo de sistemas químicos con funciones controlables a distancia.
Estos hallazgos allanan el camino para diseñar dispositivos y sensores moleculares sofisticados.

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