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Discerniendo las estructuras electrónicas e interfaciales dependientes de redox en monocapas autoensambladas
Raymond A Wong1, Yasuyuki Yokota1, Mitsuru Wakisaka2
1Surface and Interface Science Laboratory , RIKEN , 2-1 Hirosawa , Wako , Saitama 351-0198 , Japan.
Journal of the American Chemical Society
|October 3, 2018
Resumen
Este estudio revela cómo las monocapas autoensambladas terminadas en ferroceno (Fc SAM) cambian electrónicamente y estructuralmente en el agua. El control electroquímico y la espectroscopia muestran el estado redox, el emparejamiento de iones y los cambios de orientación, cruciales para los sistemas que responden al redox.
Área de la Ciencia:
- Ciencias de la superficie
- La electroquímica
- Espectroscopia
Sus antecedentes:
- Las monocapas autoensambladas terminadas en ferroceno (Fc SAM) son clave en los sistemas de respuesta redox.
- Comprender sus cambios electrónicos y estructurales en solución acuosa es vital.
Objetivo del estudio:
- Investigar las modificaciones electrónicas y estructurales redox-dependientes de las Fc SAM en ambientes acuosos.
- Para correlacionar estos cambios con el control electroquímico y el análisis espectroscópico.
Principales métodos:
- Utilizando una célula electroquímica combinada con espectroscopia de fotoelectrones de rayos X y ultravioleta (EC-XPS/UPS).
- Controlar electroquímicamente las SAM Fc y sondear los cambios en el estado redox de ferroceno/ferrocenio (Fc/Fc+), el emparejamiento iónico, la orientación molecular y el grosor de la monocapa.
Principales resultados:
- Se identificaron cambios dependientes de redox en el estado Fc/Fc+, formación de pares de iones Fc+-ClO4 y orientación molecular alterada.
- Se observó una participación insignificante del agua interfacial y se confirmó la reversibilidad de la conversión de Fc+ a Fc.
- EC-UPS confirmó la oxidación de Fc+ a través de los desplazamientos orbitales moleculares más ocupados y el aumento de la función de trabajo debido a los dipolos interfaciales y la reorientación.
Conclusiones:
- El estudio proporciona una comprensión detallada del comportamiento de los Fc SAM bajo control electroquímico.
- La metodología es aplicable a una amplia gama de sistemas de respuesta redox para el esclarecimiento de la relación estructura-función.
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