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Activación de hidrógeno a temperatura ambiente por pares de Lewis frustrados semimovilizados en redes de polímeros

Matthias Trunk¹, Johannes F Teichert², Arne Thomas¹

¹Department of Chemistry, Functional Materials, Technische Universität Berlin , Hardenbergstraße 40, 10623 Berlin, Germany.

Journal of the American Chemical Society

|March 2, 2017

Resumen

Las nuevas redes de polímeros porosos imitan a los pares de Lewis frustrados (FLP). Estos materiales permiten la escisión de dihidrógeno utilizando un ácido de Lewis fuerte, ofreciendo un nuevo enfoque para aplicaciones catalíticas.

Área de la Ciencia:

Ciencias de los materiales
Química supramolecular
Catálisis

Sus antecedentes:

La química del par de Lewis frustrado (FLP) utiliza ácidos y bases de Lewis voluminosos que no pueden formar aductos clásicos, lo que permite una reactividad única.
La inmovilización de los componentes de FLP puede mejorar la estabilidad del catalizador y la reciclabilidad, que son cruciales para las aplicaciones prácticas.
Las redes de polímeros porosos ofrecen estructuras ajustables y altas superficies para albergar especies catalíticas.

Objetivo del estudio:

Sintetizar nuevas redes de polímeros porosos que incorporen motivos de trifenilfosfina estéricamente cargados.
Investigar la formación y las propiedades de pares de Lewis frustrados semi-inmovilizados (FLPs) utilizando estas redes.
Evaluar la actividad catalítica de estos FLPs semimovilizados en la escisión de dihidrógeno.

Principales métodos:

Síntesis de redes de polímeros porosos a través de la polimerización de Yamamoto.
Incorporación de unidades de trifenilfosfina esterilizadas en la columna vertebral del polímero.
Interacciones de sondeo con el ácido de Lewis tris (pentafluorofenil) borano (B (C6F5) 3).

Principales resultados:

Síntesis exitosa de redes de polímeros porosos con motivos de trifenilfosfina.
Formación de FLP semimovilizados en combinación con B ((C6F5) 3)
Se ha demostrado la escisión heterolítica del dihidrógeno por los FLP semimovilizados a temperatura ambiente y baja presión.

Conclusiones:

Las redes de polímeros porosos pueden imitar efectivamente los sitios básicos de los FLPs.
Los FLP semimovilizados desarrollados muestran una activación eficiente del dihidrógeno en condiciones suaves.
Este trabajo presenta una estrategia prometedora para el diseño de catalizadores de FLP reciclables y robustos.

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