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La electrooxidación de los alcoholes catalizados por complejos de rutenio ligado con aminoalcohol
Kristen R Brownell1, Charles C L McCrory, Christopher E D Chidsey
1Department of Chemistry, Stanford University , Stanford, California 94305-5080, United States.
Journal of the American Chemical Society
|September 19, 2013
Resumen
Los catalizadores de rutenio en los electrodos de grafito oxidan eficientemente el metanol. Los complejos de rutenio-oxo sujetos a la superficie median este proceso de electrooxidación, generando formato.
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 son catalizadores efectivos de hidrogenación por transferencia.
- La electrocatálisis ofrece una ruta sostenible para las transformaciones químicas.
Objetivo del estudio:
- Para investigar la actividad electrocatalítica de los complejos de rutenio para la oxidación del alcohol.
- Para dilucidar el mecanismo de la electrooxidación del metanol mediada por especies de rutenio soportadas en la superficie.
Principales métodos:
- Fisiorción de catalizadores de rutenio en electrodos de grafito de plano de borde.
- Mediciones electroquímicas que incluyen voltametría cíclica y análisis Koutecky-Levich.
- Técnicas espectroscópicas y espectrométricas de masas para estudios mecanicistas (1H RMN, DESI-MS).
Principales resultados:
- Los catalizadores de rutenio en los electrodos de grafito exhiben actividad electrocatalítica para la oxidación del metanol.
- La electrooxidación del metanol (1,23 M) en solución tamponada (pH 11,5) muestra una corriente de inicio a 560 mV frente a NHE.
- El análisis de Koutecky-Levich indica un proceso de oxidación de cuatro electrones con una velocidad de 1,35 M−1 s−1 a 750 mV.
Conclusiones:
- Los catalizadores de hidrogenación por transferencia de rutenio inmovilizados en electrodos de grafito son electrocatalizadores activos para la oxidación del alcohol.
- La electrooxidación del metanol para formarlo está mediada por complejos de rutenio-oxo soportados en la superficie.
- Este estudio pone de relieve el potencial de los electrocatalizadores basados en rutenio para la oxidación eficiente del metanol.
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