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Rietveld refinement and activity of CO oxidation over Pd/Ce_(0.8)Zr_(0.2)O_2 catalyst prepared via a surfactant-assisted route

机译:表面活性剂辅助制备的Pd / Ce_(0.8)Zr_(0.2)O_2催化剂的Rietveld精制和CO氧化活性

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A surfactant-assisted preparation method was successfully used to synthesize the Ce_(0.8)Zr_(0.2)O_2 nanophases that had homogeneous chemical composition, enhanced thermal stability and improved catalytic activity. Structural refinement by the Rietveld method confirmed that many cationic lattice defects were formed in the ceria-zirconia crystals due to incorporation of the cationic surfactant in the network of the solid. Zirconium dissolving into cubic structure of ceria improved its thermal stability but led to structure distortion. FT-IR in situ characterization showed that CO chemisorption on the palladium loaded ceria-zirconia catalyst formed linear and multibonded CO-metal complexes. It was also evidenced that CO_2 was produced in the CO chemisorption procedure from the pathways of CO disproportionation and CO reacting with lattice oxygen of the catalyst. Owing to high dispersion of the loaded metal palladium and defective structure of the ceria-zirconia support, the Pd/Ce_(0.8)Zr_(0.2)O_2 catalyst calcined at a temperature range between 873 and 1173 K not only exhibited a more stable catalytic activity for CO oxidation but also performed a lower light-off temperature at cool start below 373 K in comparison with Pd/CeO_2.
机译:成功地采用表面活性剂辅助制备方法合成了具有均一的化学组成,增强的热稳定性和改善的催化活性的Ce_(0.8)Zr_(0.2)O_2纳米相。通过Rietveld方法的结构改进证实,由于在固体网络中掺入了阳离子表面活性剂,在二氧化铈-氧化锆晶体中形成了许多阳离子晶格缺陷。锆溶解在二氧化铈的立方结构中改善了其热稳定性,但导致结构变形。 FT-IR原位表征表明,钯载二氧化铈-氧化锆催化剂上的CO化学吸附形成线性和多键合的CO-金属配合物。还证明了在CO化学吸附过程中,通过CO歧化和CO与催化剂的晶格氧反应的途径产生了CO_2。由于负载的金属钯的高分散性和二氧化铈-氧化锆载体的结构不良,在873和1173 K之间的温度范围内煅烧的Pd / Ce_(0.8)Zr_(0.2)O_2催化剂不仅表现出更稳定的催化活性与Pd / CeO_2相比,它在CO氧化过程中的起燃温度更低,但在373 K以下的冷启动时起燃温度更低。

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