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Estrategia electroquímica para la instalación de relés de protones mejora la actividad de un electrocatalizador de
Shaoyang Lin1, Samragni Banerjee1, Matthew T Fortunato1
1Department of Chemistry and Biochemistry, The Ohio State University, Columbus, Ohio43214, United States.
Journal of the American Chemical Society
|October 28, 2022
Resumen
Los investigadores desarrollaron un nuevo método para la producción de hidrógeno utilizando un catalizador de rodio con un relé de protones. Este enfoque electroquímico mejora la actividad catalítica para una evolución eficiente de H2.
Área de la Ciencia:
- Química inorgánica
- La electroquímica
- Catálisis
Sus antecedentes:
- La reacción de evolución del hidrógeno (HER) es crucial para la energía sostenible.
- Los catalizadores moleculares ofrecen reactividad ajustable para HER.
- Se exploran los complejos de dirodio de rueda de remo para aplicaciones catalíticas.
Objetivo del estudio:
- Desarrollar un nuevo método para instalar un relé de protones en un complejo de dirhodium.
- Mejorar la reactividad del sitio catalítico para la producción de H2.
- Para aclarar el mecanismo de la evolución del hidrógeno asistido por protones.
Principales métodos:
- Reducción electroquímica y protonación de un complejo de dirodio.
- Voltametría cíclica (CV) y simulaciones de CV.
- Cálculos de la estructura electrónica.
- Análisis de un complejo específico: cis-[Rh2(DPhF) 2 ((bncn) 2+ (Rh-bncn).
Principales resultados:
- Se observó una preonda reversible en los CV, lo que indica una transformación precatalitica.
- La transferencia concertada de protones y electrones (CPET) en un ligando bncn inicia el proceso.
- Un enlace NH formado en el ligando bncn reducido actúa como un relé de protones.
- La evolución del hidrógeno ocurre en los ligandos puentes, no en el núcleo de dirodio.
Conclusiones:
- Se estableció una nueva estrategia de diseño para los relés de protones en electrocatalizadores HER bimetálicos.
- El método desarrollado mejora la eficiencia catalítica para la producción de H2.
- El andamio del ligando puede acomodar centros metálicos más abundantes para el desarrollo de catalizadores futuros.
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