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Naturaleza de los grupos que contienen oxígeno en el carbono para la reacción de reducción electrocatalítica de alta

Fa Yang^1,2, Xianyin Ma³, Wen-Bin Cai³

¹State Key Laboratory of Electroanalytical Chemistry, and Jilin Province Key Laboratory of Low Carbon Chemical Power , Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , 5625 Renmin Street , Changchun 130022 , P.R. China.

Journal of the American Chemical Society

|December 3, 2019

Resumen

Los nanodiscos de grafeno sin metal catalizan la reducción de CO2 para formar. Efectos sinérgicos entre los grupos carboxilo y otros grupos de oxígeno, no los grupos en solitario, actividad motriz. El rendimiento catalítico se regenera cíclicamente para una durabilidad a largo plazo.

Área de la Ciencia:

Ciencias de los materiales
La electroquímica
Catálisis

Sus antecedentes:

Los grupos que contienen oxígeno en los materiales de carbono mejoran la actividad catalítica.
La reducción electrocatalítica del dióxido de carbono (CO2RR) es crucial para la energía sostenible.
Los catalizadores sin metales ofrecen alternativas ecológicamente benignas.

Objetivo del estudio:

Investigar el papel de los grupos que contienen oxígeno en los nanodiscos de grafeno (GND) para el CO2RR.
Determinar la relación entre el contenido de grupo superficial y el rendimiento catalítico.
Desarrollar estrategias para mejorar la durabilidad del catalizador.

Principales métodos:

Síntesis de nanodiscos de grafeno de una sola capa sin metales (GND) con contenido variable de grupos de oxígeno.
Pruebas electrocatalíticas para la formación de CO2RR.
Cálculos de la teoría funcional de la densidad (DFT) para aclarar los mecanismos de reacción.
La electro-oxidación para la regeneración del catalizador.

Principales resultados:

El rendimiento de CO2RR se correlaciona positivamente con el contenido de grupo carboxilo superficial.
La alta actividad catalítica surge de los efectos sinérgicos entre los grupos carboxilo y adyacentes (hidroxilo, epoxido, carbonilo).
La regeneración cíclica de los grupos carboxilo a través de la electrooxidación restaura la actividad catalítica, asegurando la durabilidad a largo plazo.

Conclusiones:

Las interacciones sinérgicas de los grupos funcionales superficiales son clave para una alta actividad de CO2RR en GND libres de metales.
Una estrategia de "trabajo y descanso" que incluye electrooxidación permite la regeneración del catalizador y la estabilidad a largo plazo.
Este estudio proporciona información sobre las funciones de los grupos de oxígeno en la catálisis y un nuevo enfoque para el diseño de catalizadores de carbono de alto rendimiento.

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