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Dinámica y control de los sitios activos duales en polímeros de coordinación de Ni co-sustituidos para la catálisis

Yonggui Zhao¹, Nanchen Dongfang¹, Rolf Erni²

¹Department of Chemistry, University of Zurich, Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.

Journal of the American Chemical Society

|January 20, 2026

Resumen

La incorporación de cobalto en los polímeros de coordinación de níquel aumenta significativamente la cinética de la reacción de evolución del oxígeno (OER). Esta mejora se deriva de sitios activos optimizados, lo que lleva a una conversión de energía renovable eficiente y estable.

Área de la Ciencia:

Electroquímica y ciencias de los materiales
Catálisis para aplicaciones de energía renovable

Sus antecedentes:

La reacción de evolución del oxígeno (OER) es crucial para convertir la energía renovable en combustibles químicos.
Comprender la dinámica de las especies y los sitios activos durante la REA es un desafío persistente.

Objetivo del estudio:

Investigar el papel de la sustitución de cobalto (Co) en los polímeros de coordinación de níquel (Ni-CP) para el OER.
Para aclarar las ideas mecanicistas sobre cómo la incorporación de Co modula los centros de Ni y la cinética de OER.

Principales métodos:

Síntesis de Ni-CPs co-sustituidos.
Supervisión espectroscópica operando con resolución de tiempo (sensible a la superficie y a la masa).
Estudios del efecto isotópico cinético y cálculos de la teoría funcional de la densidad (DFT).

Principales resultados:

La sustitución controlada de Co genera una fracción sustancial de especies (Ni, Co) (IV), activando la formación de enlaces O-O.
Los Ni₃Co₁-CP muestran una mayor actividad OER y una estabilidad electroquímica superior (> 4000 h).
El OER procede a través de un mecanismo de acoplamiento oxo-radical con desprotonación preferente en los sitios de Ni.

Conclusiones:

La incorporación parcial de Co en Ni-CPs optimiza la geometría de coordinación local, promoviendo la cinética intrínseca de OER.
El estudio proporciona información mecanicista detallada sobre las especies activas y la dinámica de los sitios para el REA.
Los Ni₃Co₁-CP diseñados demuestran un potencial significativo para una electrocatálisis eficiente y duradera.

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