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El fotocromismo paso a paso modulado por redox en un complejo de rutenio con dietienilethene-acetilideos duales

Bin Li¹, Jin-Yun Wang, Hui-Min Wen

¹State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.

Journal of the American Chemical Society

|September 4, 2012

Resumen

Este estudio demuestra el fotocromismo gradual controlado en un nuevo complejo de rutenio (II). La investigación logró con éxito múltiples estados fotocrómicos, superando los desafíos de transferencia de energía en los sistemas de DTE.

Área de la Ciencia:

Ciencia de los materiales Ciencia de los materiales.
La fotoquímica es la fotoquímica.
Química organometálica Química orgánica de los metales.

Sus antecedentes:

Lograr el fotocromismo gradual controlado en moléculas con múltiples unidades fotocrómicas es un desafío.
La transferencia de energía entre las fracciones de dietienileteno (DTE) con anillos abiertos y cerrados puede obstaculizar la fotociclización.
Los complejos de rutenio (II) ofrecen plataformas potenciales para el desarrollo de materiales fotocrómicos avanzados.

Objetivo del estudio:

Preparar y caracterizar un nuevo complejo de rutenio ligado a bis (σ-acetiluro) (II) con dos DTE-acetiluros idénticos.
Investigar las propiedades fotocrómicas escalonadas y duales del complejo y su forma oxidada.
Para comprender la influencia del estado de oxidación del centro de rutenio en el comportamiento fotocrómico.

Principales métodos:

Síntesis y caracterización del complejo de rutenio (II) (2oo) y su forma oxidada (2oo+).
Análisis espectroscópico (NMR, UV-NIR, IR) para el seguimiento de las interconversiones fotocrómicas.
Estudios electroquímicos y computacionales para aclarar las propiedades electrónicas y los mecanismos de reacción.

Principales resultados:

Se lograron con éxito reacciones fotocrómicas graduales y duales tanto en 2oo como en 2oo+.
La banda de absorción de cierre de anillo de 2oo+ mostró un desplazamiento hacia el azul en comparación con 2oo.
La fotociclización fue más difícil en las especies oxidadas (2oo+/2co+) debido a la menor densidad electrónica en los sitios reactivos.
Se observó una interacción electrónica significativa entre las unidades DTE cerradas en el producto de cierre de doble anillo (2cc / 2cc +).

Conclusiones:

El estudio demostró con éxito el fotocromismo gradual y dual controlado en un complejo de rutenio (II).
El estado de oxidación del centro de rutenio tiene un impacto significativo en la eficiencia de la fotociclización.
Los hallazgos proporcionan información sobre el diseño de sistemas fotocrómicos multi-responsivos con propiedades sintonizables.

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