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Fluorescencia impulsada por capas en un marco orgánico covalente bidimensional

Pablo Albacete, José I Martínez¹, Xing Li²

¹Departamento de Nanoestructuras, Superficies, Recubrimientos y Astrofı́sica Molecular , Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC) , 28049 Madrid , Spain.

Journal of the American Chemical Society

|September 15, 2018

Resumen

Los investigadores crearon marcos orgánicos covalentes basados en iminas (COF) bidimensionales con apilamiento de capas ajustables. IMDEA-COF-1 exhibe fluorescencia en estado sólido, una primicia para los 2D-COF vinculados a la imina, debido a la disposición controlada de las unidades de pireno.

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Área de la Ciencia:

Ciencias de los materiales
Química orgánica
Química supramolecular

Sus antecedentes:

Las estructuras orgánicas covalentes (COF) son polímeros porosos cristalinos con estructuras sintonizables.
Los COF basados en imina se sintetizan a través de reacciones de condensación de Schiff.
El control de las propiedades en estado sólido de los FOC es crucial para sus aplicaciones.

Objetivo del estudio:

Para sintetizar nuevos COF basados en iminas 2D utilizando 1,6-diaminopireno (DAP) y aldehídos tritópicos.
Investigar el efecto del apilamiento de capas en las propiedades de fluorescencia de estos COF.
Demostrar el primer ejemplo de un COF 2D vinculado a iminas con emisión en estado sólido.

Principales métodos:

Las reacciones de condensación de Schiff entre el DAP y el 1,3,5-benzenetricarbaldehído (BTCA) o el 2,4,6-triformilfloroglucinol (TP).
Caracterización de las COF resultantes (IMDEA-COF-1 y IMDEA-COF-2) mediante técnicas como la difracción de rayos X.
Espectroscopia de fotoluminiscencia para determinar las propiedades de emisión.
Cálculos teóricos para racionalizar las estructuras de embalaje.

Principales resultados:

Formación de dos COFs basados en iminas 2D, el IMDEA-COF-1 y el IMDEA-COF-2.
Observación de fluorescencia significativa impulsada por el empaquetado de capas en estado sólido.
El apilamiento controlado de capas (eclipsado o escalonado) se logra mediante el diseño químico.
IMDEA-COF-1 exhibió una emisión verde con un rendimiento cuántico de fotoluminiscencia absoluto del 3,5%.
Los cálculos teóricos apoyaron las preferencias de embalaje observadas.

Conclusiones:

El estudio sintetizó con éxito dos nuevos COF basados en iminas 2D con fluorescencia ajustable en estado sólido.
El apilamiento controlado de capas es un factor clave para lograr las propiedades fotofísicas deseables en los FOC.
IMDEA-COF-1 representa un avance significativo como el primer 2D-COF vinculado a la imina con emisión en estado sólido.