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Posibilidades y limitaciones en las combinaciones de monómeros para marcos orgánicos covalentes bidimensionales

Mitsuharu Suzuki¹, Masashi Miura¹, Enzo Ohkubo¹

¹Division of Applied Chemistry, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.

Journal of the American Chemical Society

|January 30, 2023

Resumen

Las combinaciones de monómeros para marcos orgánicos covalentes complejos (COF) son viables si minimizan la tensión conformacional. Este hallazgo aclara el diseño de COF multicomponente y permite una diferenciación precisa entre los conjuntos de monómeros permitidos y no permitidos.

Área de la Ciencia:

Ciencias de los materiales
Química de los polímeros
Química supramolecular

Sus antecedentes:

Los marcos orgánicos covalentes (COF) ofrecen propiedades sintonizables a través de la incorporación de diversos monómeros.
El aumento de los tipos de monómeros en los COF aumenta la complejidad, pero complica la síntesis y la comprensión de la viabilidad.
La formación de COF ternarios o de mayor aridad sigue siendo un desafío debido a la incompatibilidad no clara de los monómeros.

Objetivo del estudio:

Investigar los factores primarios que rigen la viabilidad de los conjuntos de monómeros en la síntesis de COF multicomponentes.
Para aclarar el papel de la tensión conformacional frente a los factores cinéticos en la formación de COF.
Proporcionar directrices para el diseño exitoso de COF multicomponentes mediante la identificación de combinaciones viables de monómeros.

Principales métodos:

Examen sistemático de 12 combinaciones de monómeros de dos nodos y un enlace ([2 + 1]).
Análisis de los arreglos de monómeros y de las estructuras estructurales resultantes.
Evaluación de la cristalinidad del marco y de la pureza de fase.

Principales resultados:

La viabilidad del conjunto de monómeros en los COF [2 + 1] está dictada predominantemente por la tensión conformacional, no por diferencias cinéticas.
La alta tensión conformacional conduce a arreglos de monómeros desordenados, lo que resulta en COF mixtos o polímeros amorfos.
Los pares de enlaces de nodos que fallan en los COF binarios pueden formar marcos de una sola fase cuando se agrega un tercer componente.

Conclusiones:

La tensión conformacional es el determinante crítico para la formación exitosa de COF multicomponente.
La comprensión y la mitigación de la tensión son fundamentales para el diseño de FOC complejos de una sola fase.
Este trabajo proporciona un marco para predecir y lograr síntesis viables de COF multicomponentes.

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