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Electrorreducción altamente eficiente de CO2 a etanol a través del acoplamiento asimétrico C-C por un marco

Zhen-Hua Zhao¹, Jia-Run Huang¹, Pei-Qin Liao¹

¹MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, GBRCE for Functional Molecular Engineering, School of Chemistry, IGCME, Sun Yat-Sen University, Guangzhou 510275, China.

Journal of the American Chemical Society

|November 28, 2023

Resumen

Los investigadores desarrollaron un nuevo marco metálico-orgánico, CuSn-HAB, para mejorar la reacción electroquímica de reducción de CO2 (eCO2RR) para producir combustibles líquidos. Este catalizador convierte eficientemente el CO2 en alcoholes de alta selectividad y estabilidad.

Área de la Ciencia:

Ciencias de los materiales
La electroquímica
Catálisis

Sus antecedentes:

La reacción electroquímica de reducción de CO2 (eCO2RR) es crucial para la producción sostenible de combustible.
La síntesis selectiva de oxigenados multicarbónicos a través de eCO2RR es un desafío debido al acoplamiento lento C-C.
Los catalizadores heterometálicos ofrecen potencial para una mayor actividad catalítica y selectividad.

Objetivo del estudio:

Diseñar y sintetizar un nuevo marco metálico-orgánico (CuSn-HAB) con sitios duales heterometálicos.
Para investigar el rendimiento catalítico de CuSn-HAB para eCO2RR a los alcoholes.
Aclarar el mecanismo subyacente a la mayor selectividad para el acoplamiento C-C.

Principales métodos:

Síntesis de un nuevo marco metálico-orgánico (CuSn-HAB) con sitios duales de Sn·Cu.
Evaluación electroquímica del CuSn-HAB para la reducción de CO2, incluidas las mediciones de la eficiencia Faradaic y la densidad de corriente.
Estudios mecanicistas operando para comprender las vías de formación y reacción intermedias.

Principales resultados:

CuSn-HAB logró una alta eficiencia Faradaic del 56% para la producción de alcohol a -0.57 V (vs RHE).
El catalizador demostró una excelente estabilidad, sin degradación significativa durante 35 horas de funcionamiento.
Los estudios mecanicistas revelaron que los sitios duales de Sn··Cu facilitan la formación del intermediario *OCH2 y promueven el acoplamiento asimétrico C-C.

Conclusiones:

Los sitios duales heterometales Sn··Cu en CuSn-HAB superan efectivamente las limitaciones del acoplamiento lento C-C en eCO2RR.
El CuSn-HAB es un catalizador prometedor para la conversión electroquímica selectiva y estable del CO2 en alcoholes valiosos.
Este trabajo proporciona información sobre el diseño de catalizadores avanzados para una utilización eficiente del CO2.

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