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Transferencia rápida de protones y reactividad de la evolución del hidrógeno mediada por [Co₁₃ C₂

Cody R Carr¹, Atefeh Taheri¹, Louise A Berben¹

¹Department of Chemistry, University of California at Davis, Davis, California 95616, United States.

Journal of the American Chemical Society

|June 24, 2020

Resumen

Este estudio introduce un catalizador de clúster de cobalto-carbono que acelera significativamente las reacciones de transferencia de protones (PT) y transferencia de electrones (ET). Su estructura electrónica única permite velocidades de reacción de difusión limitada, superando a los métodos tradicionales.

Área de la Ciencia:

La electroquímica
Catálisis
Ciencias de los materiales

Sus antecedentes:

Los catalizadores moleculares a menudo usan relés de protones para mejorar las tasas de transferencia de protones (PT).
Los electrocatalizadores heterogéneos facilitan la transferencia concertada de electrones (ET) y PT a través del mecanismo de Volmer.
El desarrollo de catalizadores eficientes para PT y ET rápidos es crucial para varios procesos químicos.

Objetivo del estudio:

Para investigar las capacidades de transferencia de protones (PT) del cúmulo [Co13C2(CO) 24].
Determinar las velocidades de reacción y los mecanismos subyacentes de PT y ET para este catalizador.
Comparar el rendimiento catalítico con los sistemas moleculares y heterogéneos existentes.

Principales métodos:

Caracterización electroquímica del cúmulo [Co13C2...] en presencia y ausencia de protones.
Análisis cinético para determinar las tasas de transferencia de electrones (ET) y de protones (PT).
Comparación del comportamiento de difusión con nanomateriales y fullerenos.

Principales resultados:

El cúmulo [Co13C2(CO) 24] - muestra una tasa de PT notablemente alta de 2,3 × 10 ^ 9 M ^ -1 s ^ 1, lo que indica una cinética limitada por difusión.
Las ET y PT rápidas se atribuyen a la estructura electrónica deslocalizada del grupo de cobalto-carbono.
Los datos electroquímicos muestran cinética ET y comportamiento de difusión análogo a pequeños grupos, nanomateriales y fullerenos.

Conclusiones:

El cúmulo [Co13C2(CO24]4- actúa como un catalizador altamente eficiente para la transferencia de protones (PT).
Su estructura electrónica deslocalizada facilita la rápida transferencia concertada de electrones (ET) y PT.
Este grupo demuestra el potencial como una alternativa superior a los catalizadores convencionales para las reacciones electroquímicas.

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