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Influence of Solid Solution Formation on the Activity of CeO2 Supported Ni-Cu Mixed Oxide Catalysts in Dry Reforming of Methane

机译:固体溶液形成对甲烷干燥重整的CeO2负载镍锌混合氧化物催化剂的影响

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摘要

A series of CeO2 supported 20 wt% Ni-Cu mixed oxide catalysts was prepared by co-impregnation, varying the Ni-Cu composition. The catalysts were characterized by nitrogen adsorption for BET surface area, X-ray diffraction (XRD), Temperature programmed reduction (TPR), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), Transmission electron microscopy (TEM), H-2 Chemisorption, Scanning electron microscopy (SEM) and CHNS analysis techniques. They were evaluated for dry reforming of methane to produce syngas in the temperature range of 600-800 degrees C and at a GHSV=28,800h(-1). 5wt% Ni+15wt% Cu/CeO2 displayed superior activity among the series. The incorporation of Ni metal in CeO2 lattice led to the formation of Ni-O-Ce solid solution up to 5wt% Ni in the catalyst. This catalyst also showed good stability due to less coke formation. Resistance towards coking was observed to be mainly due to the abundance of labile oxygen in the solid solution.Graphical Abstract Ni incorporation in CeO2 results in significant change in the CeO2 lattice leading to solid solution formation and enhancing metal dispersion. Increase in the oxygen storage capacity (OSC) with the addition of Cu helps improve catalyst stability.
机译:通过共浸渍制备一系列支持的20wt%Ni-Cu混合氧化物催化剂,改变Ni-Cu组合物。催化剂的特征在于BET表面积,X射线衍射(XRD),温度编程(TPR),拉曼光谱,X射线光电子谱(XPS),透射电子显微镜(TEM),H-2化学吸附的氮吸附剂,扫描电子显微镜(SEM)和CHN分析技术。评估它们的甲烷干燥重整,在600-800℃的温度范围内产生合成气,在GHSV = 28,800h(-1)。 5wt%ni + 15wt%cu / ceo2在系列中显示出优异的活动。在CeO2晶格中掺入Ni金属导致催化剂中最高可达5wt%Ni的Ni-O-Ce固溶体的形成。由于较少的焦炭形成,该催化剂也显示出良好的稳定性。观察到对焦化的抵抗力主要是由于固体溶液中的不稳定氧气的丰富源性。图中,CEO2中的摘要NI掺入导致CEO2晶格的显着变化,导致固溶体形成和增强金属分散体。加入Cu的氧气储存能力(OSC)增加有助于提高催化剂稳定性。

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