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Autoensamblaje controlado, isomerismo y admisión/liberación de huéspedes de jaulas octaédricas de lantánidos
Li-Peng Zhou1, Xiao-Shan Feng1, Shao-Jun Hu1
1State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, P. R. China.
Journal of the American Chemical Society
|August 7, 2023
Resumen
Este estudio introduce jaulas orgánicas de lantánidos reversibles de carga que pueden unirse selectivamente a los huéspedes en función de su carga. Estos materiales supramoleculares adaptables ofrecen potencial para el desarrollo de sistemas inteligentes con propiedades sintonizables.
Área de la Ciencia:
- Química supramolecular
- Química de coordinación
- Ciencias de los materiales
Sus antecedentes:
- La regulación de la carga es vital para los sistemas moleculares y supramoleculares.
- El desarrollo de anfitriones de coordinación con control de carga ortogonal sigue siendo un desafío.
Objetivo del estudio:
- Informar sobre el autoensamblaje dependiente de la condición de las jaulas tetraédricas de lantánidos orgánicos con carga reversible.
- Para explorar el isomerismo y las propiedades anfitrión-invitado de estas nuevas jaulas.
- Para investigar su potencial en el desarrollo de materiales supramoleculares inteligentes.
Principales métodos:
- Autoensamblaje de iones lantánidos (Ln = Lu, Yb, Eu) con un ligando de acilhidrazona tetradentado tritópico (H6L).
- Control de la carga de la jaula a través de la desprotonación dependiente del pH del ligando.
- Caracterización mediante difracción de un solo cristal de rayos X.
- Estudios de unión huésped-huésped con huéspedes aniónicos y catiónicos.
- Estudios fotofísicos de las jaulas basadas en Yb.
Principales resultados:
- Se han sintetizado con éxito las jaulas de carga reversible [Ln6(H3L) ]6+ y [Ln6L4]6-.
- Se logra la formación exclusiva de jaulas racémicas mediante autoensamblaje y desprotonación controlados.
- Se ha demostrado la unión selectiva de sulfonatos aniónicos por jaulas catiónicas y de huéspedes de amonio por jaulas aniónicas.
- Se han observado emisiones NIR sensibilizadas a la luz visible y mejoradas por la encapsulación de huéspedes en jaulas Yb.
Conclusiones:
- Las jaulas orgánicas de lantánidos desarrolladas exhiben carga ajustable y unión selectiva de huéspedes.
- La absorción y liberación de huéspedes desencadenadas por ácido/base son factibles debido a la reversibilidad de la carga.
- Estas jaulas representan candidatos prometedores para materiales supramoleculares inteligentes con aplicaciones en detección y catálisis.
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