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Dobles hélices supramoleculares de pequeñas moléculas simétricas agrupadas en agua

René P M Lafleur¹, Svenja Herziger^2,3, Sandra M C Schoenmakers¹

¹Institute for Complex Molecular Systems, Eindhoven University of Technology, PO Box 513, Eindhoven 5600 MB, The Netherlands.

Journal of the American Chemical Society

|September 16, 2020

Resumen

Los investigadores descubrieron que las benceno-1,3,5-tricarboxamidas (BTA) forman fibras supramoleculares de doble hélice en el agua, lo que desafía los modelos anteriores de apilamiento en 1D. La composición del copolímero permite ajustar el tono helicoidal para estas nanoestructuras.

Área de la Ciencia:

Química supramolecular
Ciencias de los materiales
Nanotecnología

Sus antecedentes:

Las fibras supramoleculares son nanoestructuras clave para usos biomédicos, formadas por moléculas anfifílicas de autoensamblaje.
Estudios recientes sugieren estructuras helicoidales en forma racémica, aunque no se comprenden completamente.
Los benceno-1,3,5-tricarboxamidas (BTA) son moléculas solubles en agua utilizadas en la investigación de polímeros supramoleculares.

Objetivo del estudio:

Investigar el autoensamblaje de BTAs solubles en agua en polímeros supramoleculares.
Caracterizar la estructura de estos polímeros, abordando específicamente la formación de estructuras helicoidales.
Explorar la adaptabilidad de los parámetros estructurales, como el paso helicoidal, a través de la composición del copolímero.

Principales métodos:

Síntesis de (co) polímeros supramoleculares basados en el benceno-1,3,5-tricarboxamidas (BTA).
Microscopía electrónica de transmisión criogénica (cryo-TEM) para imágenes de alta resolución.
Reconstrucciones tridimensionales de volumen para analizar estructuras helicoidales y repeticiones.

Principales resultados:

Las BTA se autoensamblan en fibras supramoleculares de doble hélice en el agua, no en simples pilas 1D.
Se observaron repeticiones helicoidales con pitches que oscilaban entre 15 y 30 nm.
El paso helicoidal es ajustable ajustando la proporción de diferentes monómeros de BTA en copolímeros.
La formación de dimeros se propone como un mecanismo para el blindaje hidrofóbico, promoviendo la formación de doble hélice.

Conclusiones:

Los polímeros supramoleculares de BTA forman estructuras de doble hélice termodinámicamente estables en el agua.
Los hallazgos desafían la visión de larga data del apilamiento molecular 1D en tales fibras.
El análisis estructural detallado es crucial para comprender la disposición molecular precisa en las fibras supramoleculares 1D.

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