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Evolución de hidrógeno electrocatalítico ligando-centrado propuesto y oxidación del hidrógeno en un no inocente
Andrew Z Haddad1, Davinder Kumar1, Kagna Ouch Sampson1
1Department of Chemistry, University of Louisville, 2320 South Brook Street, Louisville, Kentucky 40292, United States.
Journal of the American Chemical Society
|July 11, 2015
Resumen
Este estudio detalla un complejo de renio (ReL3) que actúa como un electrocatalisador para la evolución del hidrógeno y la oxidación. Convierte eficientemente los ácidos en H2 y oxida H2 en presencia de una base.
Área de la Ciencia:
- Química Inorgánica La Química Inorgánica es la química inorgánica.
- La electrocatálisis por electrocatálisis.
- Química organometálica Química orgánica de los metales.
Sus antecedentes:
- Los complejos mononucleares de metal-tiolato son cruciales en la catálisis.
- Comprender los mecanismos de evolución y oxidación del hidrógeno es vital para las aplicaciones energéticas.
Objetivo del estudio:
- Para investigar la actividad electrocatalítica del no inocente, coordinadamente saturado mononuclear metal-tiolato complejo ReL3.3.
- Para dilucidar el mecanismo de la evolución del hidrógeno y la oxidación catalizada por ReL3.
Principales métodos:
- Estudios electroquímicos en el diclorometano.
- Análisis cinético que incluye la dependencia de la concentración de ácido y mediciones del efecto del isótopo cinético.
- Cristalografía de rayos X para determinar la estructura de los intermediarios clave.
Principales resultados:
- ReL3 cataliza la evolución del hidrógeno a partir de ácidos con un sobrepotencial de 380 mV y una frecuencia de giro de 32 ± 3 s.
- La reacción exhibe dependencia de segundo orden en la concentración de ácido y un efecto de isótopo cinético de 9 ± 1.
- ReL3 cataliza la oxidación del hidrógeno con una frecuencia de rotación de 4 ± 1 s(-1) en presencia de una base.
- Se determinó la estructura cristalina de las especies monoprotonadas [Re(LH) L2](+).
Conclusiones:
- ReL3 funciona como un electrocatalizador versátil tanto para la evolución del hidrógeno como para la oxidación.
- Se propone un mecanismo centrado en los ligandos, distinto de las vías de los hidruros metálicos, para los ciclos catalíticos.
- La especie monoprotonada es un intermediario clave en ambos procesos catalíticos.
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