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Sitios activos para la hidrogenación de CO2 a metanol en catalizadores de Cu/ZnO

Shyam Kattel¹, Pedro J Ramírez², Jingguang G Chen^3,4

¹Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA.

Science (New York, N.Y.)

|March 25, 2017

Resumen

Este estudio compara los catalizadores ZnCu y ZnO/Cu para la síntesis de metanol a partir de la hidrogenación de dióxido de carbono (CO2). Los resultados muestran que el ZnCu se oxida a ZnO, coincidiendo con la actividad ZnO/Cu, destacando la sinergia de la interfaz Cu-ZnO.

Área de la Ciencia:

Ciencias de la catálisis
Ciencias de los materiales
Ingeniería química

Sus antecedentes:

Se discuten los sitios activos para la hidrogenación de dióxido de carbono (CO2) a metanol sobre catalizadores Cu/ZnO/Al2O3.
Los principales sitios propuestos incluyen sitios bimetálicos Zn-Cu y sitios interfaciales ZnO-Cu.

Objetivo del estudio:

Para comparar directamente la actividad de los catalizadores modelo ZnCu y ZnO/Cu para la síntesis de metanol.
Para aclarar el papel de los sitios activos en la hidrogenación de CO2 al metanol.

Principales métodos:

Espectroscopia de fotoemisión de rayos X (XPS) para la caracterización de la superficie.
Teoría funcional de la densidad (DFT) para cálculos de la estructura electrónica.
Simulaciones cinéticas de Monte Carlo (KMC) para el análisis de la vía de reacción.

Principales resultados:

Los resultados experimentales y teóricos indican que los catalizadores de ZnCu se someten a oxidación superficial en condiciones de reacción.
El Zn de superficie se transforma en ZnO, lo que permite a los catalizadores ZnCu lograr la actividad de los catalizadores ZnO/Cu con una cobertura equivalente de Zn.
Se identificó un efecto sinérgico entre Cu y ZnO en la interfaz.

Conclusiones:

Los sitios activos para la síntesis de metanol implican una sinergia entre Cu y ZnO en la interfaz.
La transformación de ZnCu en ZnO/Cu en condiciones de reacción explica la actividad catalítica observada.
Los intermediarios de formato juegan un papel crucial en la vía de síntesis del metanol facilitada por la interfaz Cu-ZnO.

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