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Controlar el reconocimiento y la reactividad de los huéspedes de alquilo amonio utilizando una jaula tetraédrica

Wenyao Zhang¹, Dong Yang¹, Jie Zhao¹

¹Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education, College of Chemistry and Materials Science , Northwest University , Xi'an 710069 , China.

Journal of the American Chemical Society

|March 28, 2018

Resumen

Los investigadores desarrollaron un nuevo ligando C3-simétrico tris-bis-urea que se autoensambla con aniones de fosfato en una jaula tetraédrica altamente eficiente. Esta jaula supramolecular controla con precisión las reacciones de las moléculas huéspedes, lo que demuestra aplicaciones avanzadas de química huésped-huésped.

Área de la Ciencia:

Química supramolecular
Química entre anfitrión y huésped
Ciencias de los materiales

Sus antecedentes:

Las estructuras enjauladas son vitales en la encapsulación y catálisis del huésped.
Las jaulas basadas en metal han sido predominantes, pero las jaulas de coordinación aniónica ofrecen nuevas posibilidades.
Los conjuntos supramoleculares emergentes muestran propiedades únicas de huésped.

Objetivo del estudio:

Informar de un nuevo ligando C3-simétrico de tris-bis-urea.
Para investigar el autoensamblaje de este ligando con aniones de fosfato en una jaula tetraédrica.
Para explorar las propiedades anfitrión-invitado de la jaula y aplicaciones catalíticas.

Principales métodos:

Síntesis de un ligando tris-bis ((urea) simétrico C3 utilizando un espaciador de 2,4,6-trifenilo-1,3,5-triazina.
Autoensamblaje del ligando con aniones fosfato para formar una jaula tetraédrica de tipo A4L4.
Análisis estructural y estudios de encapsulación del huésped, incluida la metilación de DABCO.

Principales resultados:

Formación de un complejo de aniones ligando-fosfato C3-simétrico tris-bis-urea (jaula A4L4).
Se obtienen coeficientes de embalaje excepcionalmente altos (hasta el 99,5%).
Se ha demostrado la capacidad de ajuste del tamaño y la forma de la jaula (136216 Å3) a través de la flexión del plano del ligando.
Se ha controlado con éxito la metilación de DABCO, aislando limpiamente el producto monometilado.

Conclusiones:

Se sintetizó con éxito una nueva jaula basada en la coordinación aniónica con propiedades sintonizables.
La jaula exhibe una alta eficiencia en la encapsulación del huésped y un control preciso de las reacciones del huésped.
Este trabajo amplía el alcance de las jaulas supramoleculares para aplicaciones avanzadas en catálisis y reconocimiento molecular.

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