Effect of the presence of CuOx on the catalytic behavior of bimetallic Au-Cu catalyst supported on Ce-Zr mixed oxide in CO preferential oxidation
Influencia de la presencia de CuOx sobre el comportamiento catalítico de un catalizador bimetálico Au-Cu soportado en óxido mixto Ce-Zr en la oxidación preferencial de CO
DOI:
https://doi.org/10.15446/ing.investig.v39n2.76586Keywords:
Preferential oxidation of CO, Nano-gold particles, Copper, Mixed oxide (en)Oxidación preferencial de CO, Nanopartículas de oro, Cobre, Óxido mixto (es)
The effect of the presence of copper was evaluated on a bimetallic catalyst Au-Cu based on mixed oxide cerium-zirconium in the preferential oxidation of CO (CO-PROX). Six catalytic materials, based on mixed oxides, were prepared: (1) the support (CeZr); (2) the monometallic catalysts, i.e. gold (Au/CeZr), (3) impregnated copper oxide (CuOx/CeZr) and (4) incorporated copper (CuCeZr); and the bimetallic catalysts, i.e. (5) impregnated copper oxide and gold (Au-CuOx/CeZr), and (6) gold and incorporated copper (Au/CuCeZr). The catalysts were evaluated in the CO-PROX in the range 30-300°C and atmospheric pressure, where the Au-CuOx/CeZr showed the best catalytic behavior. The influence of CO2 and H2O in the feed stream was evaluated on the catalytic performance of the Au-CuOx/CeZr. An inhibitory effect for the CO2 was observed, while the presence of H2O enhanced the performance. Additionally, the catalytic stability was evaluated, reaching CO conversion of 93% and selectivity of 90% for 118 h. The catalytic materials were characterized by XRD, showing in all cases the fluorite cubic structure. The N2 adsorption-desorption analyses showed that synthesized materials were mesoporous and the TPR-H2 test reveals that the presence of the active phase increases the reducibility of Ce4+ to Ce3+. Reduction peaks of the gold catalyst were present at lower temperatures than those of the copper catalyst, which is related to a hydrogen spillover phenomenon. Finally, the samples were analyzed by SEM and TEM, which confirmed the formation of nano-particles with a diameter of about 4 nm.
la oxidación preferencial de CO (CO-PROX). Se prepararon seis materiales catalíticos: (1) el soporte (CeZr); los catalizadores monometálicos que fueron (2) oro (Au/CeZr), (3) cobre impregnado (CuOx/CeZr) y (4) cobre incorporado (CuCeZr); y los catalizadores bimetálicos que fueron (5) óxido de cobre impregnado y oro (Au-CuOx/CeZr), y (6) oro y cobre incorporado (Au/CuCeZr). Los catalizadores se evaluaron en el CO-PROX en un rango de temperaturas de 30-300°C y presión atmosférica, donde el Au-CuOx/CeZr mostró el mejor desempeño catalítico. Se evaluó la influencia de CO2 y H2O en la mezcla de alimento sobre el desempeño del catalizador Au-CuOx/CeZr, donde se observó un efecto inhibitorio del CO2, mientras que la presencia del agua mejoró el desempeño. Adicionalmente, se evaluó la estabilidad catalítica, la cual alcanzó conversiones de CO de 93% con una selectividad de 90%, durante 118 h. Los materiales catalíticos se caracterizaron por DRX, presentando en todos los casos la estructura fluorita cúbica. Las pruebas de adsorción y desorción de N2 mostraron que los materiales sintetizados eran mesoporosos. Los ensayos de TPR-H2, mostraron que la presencia de la fase activa incrementó la reducibilidad de Ce4+ a Ce3+. Los picos de reducción del catalizador de oro se presentaron a temperaturas más bajas con respecto al catalizador de cobre, lo cual se relaciona con el fenómeno spillover para el hidrógeno. Finalmente, las muestras se analizaron por SEM y TEM, las cuales confirmaron la formación de nanopartículas con un diámetro alrededor de 4nm.
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1. Zhengling Li, Hao Cheng, Xuebin Zhang, Mao Ji, Shuyao Wang, Shudong Wang. (2021). CuW/CeZr Catalysts: A Dual-Function Catalyst for Selective Catalytic Reduction of NO and CO Oxidation Under Oxygen-Rich Conditions. Catalysis Letters, 151(11), p.3361. https://doi.org/10.1007/s10562-021-03562-3.
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