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Intercambio de plantilla oscilatoria en cápsulas de polioxometalato: una oscilación activada por ligando, impulsada

Haralampos N Miras¹, Marjorie Sorus, Jonathan Hawkett

¹WestCHEM, School of Chemistry, The University of Glasgow, Glasgow G12 8QQ, United Kingdom.

Journal of the American Chemical Society

|April 11, 2012

Resumen

Se observaron oscilaciones controladas por redox entre los aniones fosfato y vanadato dentro de los grupos {X(2) M(18) }. Se lograron seis ciclos completos utilizando el agente reductor de TEA, lo que demuestra el intercambio aniónico dinámico en la química del polioxometalato.

Área de la Ciencia:

Química Inorgánica La Química Inorgánica es la química inorgánica.
Química supramolecular de las moléculas.
Química de los polioxometalatos La química de los polioxometalatos

Sus antecedentes:

Los polioxometalatos (POM) son grupos inorgánicos versátiles con propiedades sintonizables.
El intercambio de aniones impulsado por plantillas es un mecanismo clave para la funcionalización de los POM.
El comportamiento oscilatorio en los sistemas POM es raro y poco explorado.

Objetivo del estudio:

Para investigar el intercambio de plantilla oscilatoria controlada por redox entre los aniones fosfato (P) y vanadato (V).
Para caracterizar la interconversión dinámica de las especies {P} y {V} dentro de una cápsula POM.
Para determinar las condiciones necesarias para el comportamiento oscilatorio sostenido.

Principales métodos:

Espectrometría de masas de ionización por electrospray correlacionada (ESI-MS) para la identificación de especies.
Espectroscopia de resonancia paramagnética de electrones (EPR) para el monitoreo del estado redox.
Espectroscopia ultravioleta visible (UV-vis) para el seguimiento de los cambios espectrales en el tiempo.
Análisis cinético de las reacciones de intercambio aniónico.

Principales resultados:

Se ha demostrado el intercambio exitoso de plantilla oscilatoria entre aniones fosfato y vanadato dentro de un grupo {X(2) M(18) }.
Se observaron hasta seis oscilaciones completas, convirtiendo {P} en {V} y viceversa.
Identificó el agente reductor de TEA como crucial para permitir estas oscilaciones.
Cuantificó la cinética de la reacción y las concentraciones de especies a lo largo de los ciclos de oscilación.

Conclusiones:

El control de redox es una estrategia viable para inducir el comportamiento oscilatorio en los sistemas POM.
El cúmulo {X(2) M(18)} puede soportar el intercambio aniónico dinámico y reversible.
Este trabajo abre caminos para el diseño de materiales inorgánicos sensibles y dinámicos.

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