Synthesis, physicochemical and catalytic properties of Ni/PrCeZrO catalysts for water-gas shift reaction

T. Larina, Yulia Fedorova, T. Krieger, A. Ishchenko, T. Glazneva, E. Sadovskaya, N. Eremeev, V. Sadykov
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引用次数: 3

Abstract

Abstract Mixed nanocrystalline ceria-zirconia oxides doped with praseodymium containing 5, 7.5, 10, and 12.5 wt. % nickel were prepared by the incipient wetness impregnation of the oxide support. Complex physicochemical characterization by X-ray diffraction analysis, ultraviolet-visible diffuse reflectance spectroscopy, high resolution transmission electron microscopy and Fourier-transform infrared spectroscopy of adsorbed CO revealed that the nickelcontaining samples are comprised of a solid solution of praseodymium, cerium and zirconium oxides with the fluorite structure as well as nickel oxide particles with a size up to 100 nm. All prepared nanocomposite catalysts show a high catalytic activity in the water-gas shift reaction. The optimum content of nickel in the catalyst providing the maximum activity was found to be 10 wt. %. A high oxygen mobility in these catalysts estimated by the temperature-programmed oxygen isotope heteroexchange with C18O2 provides required coking stability. To eliminate local overheating of the catalyst and decrease the pressure drop in the reactor, as required for further up-scaling, the active component was supported on a metal plate made of Ni-Al foam alloy. At a fixed contact time, the same level of CO conversion with a fraction of the active component was achieved with an approximately 50 wt% loading on the support.
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Ni/PrCeZrO水气转换催化剂的合成、理化性质及催化性能研究
摘要采用初湿浸渍法制备了含镍量为5%、7.5%、10%和12.5 wt. %的镨掺杂的混合纳米晶氧化铈-氧化锆。通过x射线衍射分析、紫外-可见漫反射光谱、高分辨率透射电镜和傅里叶变换红外光谱对吸附CO进行了复杂的理化表征,发现含镍样品由具有萤石结构的氧化镨、氧化铈和氧化锆固溶体以及尺寸达100 nm的氧化镍颗粒组成。所制备的纳米复合催化剂在水气转换反应中表现出较高的催化活性。催化剂中镍的最佳含量为10 wt. %,可提供最大活性。通过与C18O2的程序化氧同位素异质交换,这些催化剂的高氧迁移率提供了所需的焦化稳定性。为了消除催化剂的局部过热和降低反应器中的压降,根据进一步放大的需要,活性组分被支撑在镍铝泡沫合金制成的金属板上。在固定的接触时间内,在支架上大约50 wt%的负荷下,用一小部分活性成分实现了相同水平的CO转化。
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