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Redes dinámicas constitucionales de orden superior: Redes [2×3] y [3×3] que muestran una adaptación jerárquica

Guangwen Men^1,2, Jean-Marie Lehn¹

¹Laboratoire de Chimie Supramoléculaire, Institut de Science et d'Ingénierie Supramoléculaires (ISIS), Université de Strasbourg , 8 allée Gaspard Monge, 67000 Strasbourg, France.

Journal of the American Chemical Society

|February 2, 2017

Resumen

Este estudio explora las redes dinámicas constitucionales complejas (CDN) utilizando bibliotecas covalentes dinámicas (DCL) con estructuras de orden superior. Los investigadores observaron nuevos comportamientos adaptativos y salidas más simples del aumento de la complejidad del sistema.

Área de la Ciencia:

Química supramolecular
Biología de los sistemas químicos
Ciencias de los materiales

Sus antecedentes:

Las bibliotecas covalentes dinámicas (DCL) son sistemas de moléculas que pueden reorganizarse a través de enlaces covalentes reversibles.
Las redes dinámicas constitucionales (CDN) representan el equilibrio dinámico de los componentes dentro de las DCL.
La extensión de las CDN más allá de las arquitecturas simples [2x2] es crucial para desarrollar materiales adaptativos más sofisticados.

Objetivo del estudio:

Para investigar las redes dinámicas constitucionales de orden superior (CDN [2x3] y [3x3]) basadas en bibliotecas covalentes dinámicas.
Analizar las respuestas adaptativas de estas CDN complejas a estímulos de efector único y múltiple.
Demostrar la prueba de principio utilizando ligandos orgánicos dinámicos y efectores de cationes metálicos.

Principales métodos:

Diseño y síntesis de bibliotecas covalentes dinámicas [2x3] y [3x3] utilizando hidrazona, acilhidrazona y ligandos de imina.
Aplicación de efectores de cationes metálicos únicos y múltiples (Cu+, Zn2+, Fe2+) para estudiar las respuestas de la red.
Análisis de las interconversiones y comportamientos adaptativos, incluida la amplificación agonista y las respuestas jerárquicas.

Principales resultados:

Generación exitosa de CDN [2x3] con estructuras prismáticas trigonales y respuestas específicas a los efectores Cu+ y Zn2+, mostrando doble amplificación agonista.
Diseño de CDN más complejas [3x3] con nueve constituyentes de ligandos, que exhiben nuevos comportamientos adaptativos como subredes y amplificación agonística diagonal.
Demostración de respuestas dependientes de la secuencia a los efectores, donde la aplicación jerárquica influye en la destrucción o formación de la red.
Observación de que el aumento de la complejidad del sistema puede conducir a resultados simplificados a través de la competencia de componentes dinámicos.

Conclusiones:

Las CDN de orden superior ([2x3] y [3x3]) se pueden construir a partir de DCL, exhibiendo comportamientos adaptativos complejos.
Los efectores de cationes metálicos pueden controlar con precisión las respuestas de CDN, incluidos nuevos patrones de amplificación y resultados dependientes de la secuencia.
El estudio pone de relieve el potencial de los sistemas dinámicos complejos para crear materiales y sistemas químicos adaptativos sofisticados.

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