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Desarrollo de una plataforma de electrocatálisis de película delgada tipo UiO con enlaces redox activos

Ben A Johnson¹, Asamanjoy Bhunia¹, Honghan Fei²

¹Department of Chemistry Ångström Laboratory, Uppsala University Box 523, 75120 Uppsala, Sweden.

Journal of the American Chemical Society

|February 10, 2018

Resumen

Este estudio introduce el primer marco electroactivo metal-orgánico (MOF) que utiliza enlaces redox-activos para mejorar el transporte de cargas en la electrocatálisis. El material demuestra una eficiente propagación de carga y conductividad de protones, crucial para aplicaciones electroquímicas avanzadas.

Área de la Ciencia:

Ciencias de los materiales
La electroquímica
Nanotecnología

Sus antecedentes:

Las estructuras metal-orgánicas (MOF) ofrecen una gran superficie y estructuras sintonizables para la catálisis.
El transporte eficiente de cargas es fundamental para los electrocatalizadores basados en MOF, pero sigue siendo un desafío.
El desarrollo de MOF con electroactividad intrínseca y transporte de carga/protón facilitado es esencial.

Objetivo del estudio:

Sintetizar y caracterizar el primer MOF electroactivo con topología UiO/PIZOF utilizando enlaces redox-activos.
Investigar los mecanismos de transporte de carga y la conductividad de protones dentro del MOF.
Evaluar las propiedades electrocrómicas y la actividad electroquímica de las películas delgadas de MOF.

Principales métodos:

Síntesis de Zr(dcphOH-NDI) MOF con enlaces de diimida de naftaleno redox activo (NDI).
Incorporación de grupos hidroxilo para el transporte de protones.
Fabricación de películas delgadas sobre sustratos de óxido de estaño dopados con fluor.
Las titulaciones potenciométricas, la voltametría cíclica y la electroquímica del espectro UV/Vis.

Principales resultados:

Zr ((dcphOH-NDI) exhibe un comportamiento de respuesta de protones con valores de pKa distintos.
Las películas delgadas de Zr ((dcphOH-NDI) @ FTO muestran electrocromismo reversible debido a la reducción del enlace NDI.
Se observó una alta actividad electroquímica (97%) en los sitios de NDI.
El transporte de carga ocurre a través de saltos de enlace a enlace, influenciado por el tamaño del catión electrolito.

Conclusiones:

El MOF desarrollado es el primer material electroactivo de su tipo con topología UiO/PIZOF.
El material facilita el transporte eficiente de carga y protones, adecuado para la electrocatálisis.
El mecanismo de salto de enlace a enlace y la influencia del electrolito en la difusión son hallazgos clave.

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