固相浸渍法和湿浸渍法制备CuO/CeO2催化剂及其CO氧化性能的对比研究

doi:10.1016/S1872-2067(14)60138-8

催化学报 ›› 2014, Vol. 35 ›› Issue (8): 1347-1358.DOI: 10.1016/S1872-2067(14)60138-8

固相浸渍法和湿浸渍法制备CuO/CeO₂催化剂及其CO氧化性能的对比研究

孙敬方^a, 张雷^b, 葛成艳^b, 汤常金^b, 董林^a,b

a. 南京大学现代分析中心, 江苏省机动车尾气污染控制重点实验室, 江苏南京 210093;
b. 南京大学化学化工学院, 介观化学教育部重点实验室, 江苏南京 210093

收稿日期:2014-04-03 修回日期:2014-05-05 出版日期:2014-08-01 发布日期:2014-08-05
通讯作者: 汤常金, 董林
基金资助:
国家重点基础研究发展计划（973计划，2010CB732300，2009CB623500）.

Comparative study on the catalytic CO oxidation properties of CuO/CeO₂ catalysts prepared by solid state and wet impregnation

Jingfang Sun^a, Lei Zhang^b, Chengyan Ge^b, Changjin Tang^b, Lin Dong^a,b

a. Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Nanjing University, Nanjing 210093, Jiangsu China;
b. Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu China

Received:2014-04-03 Revised:2014-05-05 Online:2014-08-01 Published:2014-08-05
Supported by:
This work was supported by the National Basic Research Program of China (973 Programs, 2009CB623500, 2010CB732300).

摘要/Abstract

摘要：

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.

关键词: 一氧化碳氧化, 氧化铜/二氧化铈, 固相浸渍法, 湿浸渍法, 协同作用机制

Abstract:

A series of CuO/CeO₂ catalysts were prepared by solid state impregnation (SSI) and wet impregnation (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 benefited the reduction of CuO species. LRS results indicated that a higher concentration of oxygen vacancies 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 counterparts 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.

Key words: Carbon monoxide oxidation, Copper oxide, Cerium oxide, Solid state impregnation, Wet impregnation, Synergistic mechanism

孙敬方, 张雷, 葛成艳, 汤常金, 董林. 固相浸渍法和湿浸渍法制备CuO/CeO₂催化剂及其CO氧化性能的对比研究[J]. 催化学报, 2014, 35(8): 1347-1358.

Jingfang Sun, Lei Zhang, Chengyan Ge, Changjin Tang, Lin Dong. Comparative study on the catalytic CO oxidation properties of CuO/CeO₂ catalysts prepared by solid state and wet impregnation[J]. Chinese Journal of Catalysis, 2014, 35(8): 1347-1358.

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固相浸渍法和湿浸渍法制备CuO/CeO₂催化剂及其CO氧化性能的对比研究

Comparative study on the catalytic CO oxidation properties of CuO/CeO₂ catalysts prepared by solid state and wet impregnation

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