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Improved reactivity for toluene oxidation on MnOx/CeO2-ZrO2 catalyst by the synthesis of cubic-tetragonal interfaces
Applied Surface Science ( IF 6.3 ) Pub Date : 2021-02-01 , DOI: 10.1016/j.apsusc.2020.148188
Caixia Zhou , Hailong Zhang , Zhun Zhang , Luming Li

Abstract In this study, the CeO2-ZrO2 solid solutions with cubic-tetragonal interfaces were prepared by an urea hydrolysis method and a solvothermal method. Then they were used as the supports and Mn/Ce-Zr catalysts were prepared by impregnation method. The catalytic performance of the catalysts for toluene oxidation were evaluated by a steady-state measurement and compared with that of Mn/Ce-Zr-ss without the interfaces, in which the support was prepared by co-precipitation. The result was found that the catalyst interfaces apparently enhanced catalytic activity for toluene oxidation. The coexistence of cubic and tetragonal phases and their interfaces were confirmed by XRD and HRTEM. H2-TPR and XPS results indicated that the cubic-tetragonal interfaces led to stronger interaction between surface Mn and Ce species and higher concentration of lattice oxygen produced from the catalyst surface. DRIFT spectra revealed that the catalyst interface promoted the adsorption of toluene and the formation of key intermediates at low temperatures. These would be important factors that caused a higher activity of the catalyst with cubic-tetragonal interfaces. Moreover, the promoting role of the interfaces might be related to the morphology, surface area and interface components of Ce-Zr supports.

中文翻译:

通过合成立方-四方界面提高甲苯氧化在 MnOx/CeO2-ZrO2 催化剂上的反应性

摘要 本研究采用尿素水解法和溶剂热法制备了立方-四方界面的CeO2-ZrO2固溶体。然后将它们用作载体并通过浸渍法制备Mn/Ce-Zr催化剂。通过稳态测量评估甲苯氧化催化剂的催化性能,并与无界面的 Mn/Ce-Zr-ss 进行比较,其中载体通过共沉淀制备。结果发现,催化剂界面明显提高了甲苯氧化的催化活性。XRD 和 HRTEM 证实了立方相和四方相的共存及其界面。H2-TPR 和 XPS 结果表明立方-四方界面导致表面 Mn 和 Ce 物种之间更强的相互作用以及催化剂表面产生的更高浓度的晶格氧。漂移光谱表明,催化剂界面促进了甲苯的吸附和低温下关键中间体的形成。这些将是导致具有立方-四方界面的催化剂具有更高活性的重要因素。此外,界面的促进作用可能与 Ce-Zr 载体的形态、表面积和界面成分有关。这些将是导致具有立方-四方界面的催化剂具有更高活性的重要因素。此外,界面的促进作用可能与 Ce-Zr 载体的形态、表面积和界面成分有关。这些将是导致具有立方-四方界面的催化剂具有更高活性的重要因素。此外,界面的促进作用可能与 Ce-Zr 载体的形态、表面积和界面成分有关。
更新日期:2021-02-01
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