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Reducción electrocatalítica de O2 por complejos de cobre mononucleares covalentemente inmovilizados: evidencia de un
Charles C L McCrory1, Anando Devadoss, Xavier Ottenwaelder
1Department of Chemistry, Stanford University, Stanford, California 94305, United States.
Journal of the American Chemical Society
|March 4, 2011
Resumen
Un nuevo electrocatalizador de cobre (I) inmovilizado en una superficie de carbono vidrioso reduce eficientemente el oxígeno al agua. Este proceso requiere dos sitios de cobre, lo que indica un mecanismo cooperativo para una mayor reducción de oxígeno.
Área de la Ciencia:
- La electroquímica es electroquímica.
- Ciencia de los materiales Ciencia de los materiales.
- La catálisis de la catálisis.
Sus antecedentes:
- La reacción de reducción de oxígeno (ORR) es crucial para la conversión de energía.
- El desarrollo de electrocatalizadores eficientes para ORR es un desafío clave.
- Los complejos de cobre son prometedores para la catálisis ORR.
Objetivo del estudio:
- Investigar la actividad electrocatalítica de un complejo de Cu (I) inmovilizado covalentemente para la reducción de oxígeno.
- Para aclarar el mecanismo de la reducción de cuatro electrones (4-e) de O(2) a H(2) O.O.
- Para comparar el rendimiento de los sistemas de Cu (I) covalentemente inmovilizados y fisicorbados.
Principales métodos:
- Inmovilización covalente de un complejo 3-etinile-fenantrolina Cu (I) sobre un electrodo de carbono vidrioso modificado con azida.
- Caracterización electroquímica del catalizador inmovilizado.
- Análisis cinético de la reacción de reducción de oxígeno.
Principales resultados:
- El complejo Cu(I) inmovilizado actúa como un electrocatalizador activo para la reducción 4-e de O(2) a H(2) O.
- La velocidad de reacción es de segundo orden con respecto a la cobertura de Cu, lo que sugiere un mecanismo de dos sitios.
- Los mecanismos propuestos son consistentes con los sistemas de Cu (I) inmovilizados y físicamente absorbidos.
Conclusiones:
- La inmovilización covalente proporciona una estrategia efectiva para el desarrollo de electrocatalizadores ORR estables y activos.
- La reducción de 4 e de O2 probablemente implica una acción cooperativa de dos centros de Cu1.
- Comprender el mecanismo es vital para el diseño de sistemas electrocatalíticos de próxima generación.
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