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Ensamblaje estereoselectivo de ruedas gigantes de molibdeno quiral utilizando iones lantánidos y aminoácidos
Weimin Xuan1, Robert Pow1, Nancy Watfa1
1WestCHEM, School of Chemistry , The University of Glasgow , Glasgow G12 8QQ , United Kingdom.
Journal of the American Chemical Society
|November 30, 2018
Resumen
Los investigadores desarrollaron un nuevo método para sintetizar grandes grupos quirales de polioxometalato (POM) utilizando lantánidos y aminoácidos. Este avance permite la creación de POMs enantiopuros con propiedades únicas de huésped y capacidad catalítica.
Área de la Ciencia:
- Química inorgánica
- Ciencias de los materiales
- Química supramolecular
Sus antecedentes:
- La síntesis de polioxometalatos intrínsecamente quirales (POM) es un desafío debido a las dificultades para controlar la quiralidad del marco metaloxo.
- Los métodos existentes a menudo tienen dificultades para inducir la asimetría necesaria para la formación de POM enantiopuro.
Objetivo del estudio:
- Para lograr una síntesis estereoselectiva de gigantescos grupos quirales de polioxometalato.
- Explorar la química huésped-huésped y las aplicaciones catalíticas de estos nuevos POMs quirales.
Principales métodos:
- Utilizó iones lantánidos coordinados como disuasores de simetría.
- Se emplean ligandos de aminoácidos para dirigir la formación de estructuras quirales.
- Caracterizó la quiralidad y la estabilidad utilizando dicroísmo circular, RMN de 1H y espectrometría de masa de movilidad de iones por electrospray.
Principales resultados:
- Sintetizó con éxito una serie de gigantescos grupos quirales de Molibdeno Azul (MB) POM ({Mo124Ce4}) con configuraciones definidas de Δ o Λ.
- Demostró la capacidad del marco quiral MB para encapsular un clúster quiral {Mo8} previamente inaccesible.
- Se demostró la transformación in situ del triptófano en cinurenina, mediada por el huésped quiral MB.
Conclusiones:
- Desarrolló una estrategia sinérgica utilizando lantánidos y aminoácidos para la síntesis estereoselectiva de POM.
- Se estableció que estos gigantescos POM quirales exhiben un potencial significativo en la química huésped-huésped y la catálisis selectiva.
- Abrió nuevas vías para el diseño de materiales inorgánicos quirales complejos con funcionalidades a medida.
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