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Oxidación electrocatalítica selectiva de un complejo re-metilo a metanol por un catalizador polipiridil de Ru (II)

Michael K Coggins¹, Manuel A Méndez, Javier J Concepcion

¹Department of Chemistry, University of North Carolina at Chapel Hill , Chapel Hill, North Carolina 27599, United States.

Journal of the American Chemical Society

|October 18, 2014

Resumen

Este estudio presenta un catalizador de rutenio (Ru) en electrodos nanoITO para la oxidación selectiva de trióxido de metilrenio (MTO) a metanol. El catalizador logra un alto rendimiento de metanol a través de un mecanismo de inserción de enlace metilo-renio propuesto.

Área de la Ciencia:

La electroquímica es electroquímica.
La catálisis es la catálisis.
Ciencia de los materiales Ciencia de los materiales.

Sus antecedentes:

Los complejos de rutenio se exploran para las reacciones de oxidación catalítica.
El desarrollo de electrocatalizadores eficientes para la conversión selectiva de sustratos es crucial.
Las películas de nanopartículas mesoporosas ofrecen una gran superficie para aplicaciones catalíticas.

Objetivo del estudio:

Para investigar la oxidación electrocatalítica del trióxido de metilrenio (MTO) al metanol.
Para caracterizar un nuevo complejo de rutenio enlazado a la superficie en electrodos nanoITO.
Para dilucidar el mecanismo de reacción y la cinética de la oxidación MTO.

Principales métodos:

Síntesis electroquímica y caracterización de los electrodos nanoITO-Ru.
Electrolisis controlada del potencial de MTO en una solución acuosa ácida.
Estudios de cinética electroquímica para determinar el orden de reacción y las constantes de velocidad.

Principales resultados:

El catalizador nanoITO-Ru ((II) ((OH2) ((2+) oxida selectivamente el MTO a metanol con un rendimiento Faradaico del 87%.
La activación oxidativa a nanoITO-Ru ((IV) ((OH) ((3+) es clave para la oxidación de MTO.
La cinética de la reacción muestra una dependencia de primer orden del MTO con la saturación de la tasa.

Conclusiones:

El electrocatalizador desarrollado demuestra una alta selectividad para la producción de metanol a partir de MTO.
Se propone un mecanismo de reacción que implica la inserción directa en el enlace renio-metilo.
El rendimiento del catalizador es dependiente del potencial, con una selectividad óptima a 1.3 V frente a NHE.

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