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Evolución dinámica y reversibilidad de un solo nanocúmulo Au25 para la reacción de reducción de oxígeno

Zehui Sun¹, Jia Wang², Lei Su¹

¹Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, PR China.

Journal of the American Chemical Society

|July 12, 2024

Resumen

Este estudio revela el comportamiento dinámico del ligando en los nanocúmulos de oro (Au25 NC) durante la reacción de reducción de oxígeno (ORR). El monitoreo en tiempo real muestra interruptores de actividad "ON-OFF", que ofrecen nuevos conocimientos sobre la catálisis de nanoclusters.

Área de la Ciencia:

Ciencia de los nanomateriales
La electroquímica
Catálisis

Sus antecedentes:

Los nanocúmulos metálicos ultrapequeños (NC) son catalizadores prometedores.
Comprender sus sitios activos dinámicos en condiciones de reacción es un desafío.

Objetivo del estudio:

Para controlar en tiempo real la actividad electrocatalítica dinámica de un solo nanocúmulo de oro protegido por ligando (Au25 NC) durante la reacción de reducción de oxígeno (ORR).
Elucidar la correlación estructura-actividad de las NC a nivel atómico.

Principales métodos:

Utilizó la electroquímica de colisión de una sola nanopartícula.
Utilizó un nanoelectrodo de carbono con cavidad.
Resultados experimentales combinados con simulaciones computacionales.

Principales resultados:

Se ha observado una despasivación y una pasivación reversibles del ligando en la superficie NC Au25.
Evolución dinámica de la conformación del núcleo Au25.
Se han detectado interruptores de corriente "ON-OFF" y fluctuaciones de "ON" durante la ORR.

Conclusiones:

La dinámica de los ligandos y los cambios en la conformación del núcleo dictan la actividad electrocatalítica de las NC Au25.
Estos hallazgos proporcionan una nueva comprensión de las relaciones estructura-actividad en la catálisis de nanoclusters.

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