采用固相浸渍法和常规湿浸渍法制备了一系列CuO/CeO2催化剂,并结合X射线衍射(XRD)、氢气-程序升温还原(H2-TPR)、激光拉曼光谱(LRS)、原位漫反射红外光谱(in situ DRIFTS)、X射线光电子能谱(XPS)等手段考察了制备方法对催化剂结构性质及其在CO氧化反应中性能的影响. XPS和H2-TPR结果表明,固相浸渍法更有利于得到高分散的铜物种,并促进CuO物种的还原. LRS结果表明,相比于湿浸渍法,固相浸渍法能产生更多氧空位,而这些氧空位可以活化参与反应的O2. CO氧化活性测试结果表明,当铜负载量相同时,固相浸渍法制备的催化剂相比于湿浸渍法表现出更好的催化性能.结合多种表征结果发现,催化剂CO氧化性能与其表面氧空位和Cu+-CO浓度紧密相关,提出了CuO/CeO2催化剂在CO氧化反应中可能的协同作用机制.
A series of CuO/CeO2 catalysts were prepared by solid state impregnation (SSI) and wet impregna-tion (WI) methods and characterized by X-ray diffraction, H2 temperature-programmed reduction (H2-TPR), laser Raman spectroscopy (LRS), in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), and X-ray photoelectron spectroscopy (XPS). XPS and H2-TPR results showed that SSI increased the dispersion of the copper species on the catalyst surface, which bene-fited the reduction of CuO species. LRS results indicated that a higher concentration of oxygen va-cancies was obtained by the SSI method unlike the WI method. CO oxidation results showed that at a given CuO loading, the activity of the catalysts prepared by SSI was higher than that of their coun-terparts prepared by WI. Based on the combined characterization results, it was suggested that the enhanced activity was closely related to the higher concentrations of oxygen vacancies and Cu+-CO species on the catalysts. Last, a possible synergetic mechanism was proposed for CO oxidation over the CuO/CeO2 catalysts.
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