制备方法对CuO-CeO2/ZrO2催化CO氧化性能的影响 |
Effect of Preparation Method on Catalytic Performance of CuO-CeO2/ZrO2 for CO Oxidation |
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摘要: 以ZrO2为载体、采用不同的浸渍次序制备了3种CuO-CeO2/ZrO2催化剂并在不同的温度(500,650和800 ℃)下进行焙烧,利用X射线衍射(XRD)、程序升温还原(H2-TPR和CO-TPR)及CO程序升温脱附(CO-TPD)技术对所制备的催化剂进行了表征,并采用色谱流动法考察了其催化CO低温氧化反应性能。结果表明,当焙烧温度为650 ℃时,3种催化剂的CO催化氧化活性均最佳,且三者的催化活性大小顺序为:CuO/CeO2/ZrO2>CuO-CeO2/ZrO2>CeO2/CuO/ZrO2。结合催化剂的表征和活性测试结果,我们认为高分散的CuO是CO的吸附中心,有利于CO的低温氧化反应,而大颗粒的CuO几乎对CO没有吸附作用,不利于CO的低温氧化反应。在3种催化剂中,CuO/CeO2/ZrO2催化剂具有最佳的低温还原特性和最大的CO2脱附峰面积,相应地具有最佳的催化氧化活性。 |
关键词: 浸渍法 CuO-CeO2/ZrO2 催化活性 CO氧化 |
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Abstract: Three types of CuO-CeO2/ZrO2 catalysts were prepared with ZrO2 as the support by different impregnation sequences, and were calcined at different temperatures (500, 650 and 800 ℃). These catalysts were characterized by X-ray diffraction (XRD), temperature-programmed reduction by H2 or CO (H2-TPR, CO-TPR), and temperature-programmed desorption of CO (TPD) techniques. Their catalytic activities for low temperature CO oxidation were investigated using a microreactor-gas chromatograph system. The results indicate that the catalytic activity for the catalysts calcined at 650 ℃ is the highest and is in the following order: CuO/CeO2/ZrO2>CuO-CeO2/ZrO2>CeO2/CuO/ZrO2. Based on the results of characterizations and catalytic activity measurements, we propose that the well-dispersed CuO is the center for adsorption of CO and is favorable for low-temperature CO oxidation, and the bulk CuO contributes little to the catalytic activity because of its inability to adsorb CO. Among the three types of catalysts, CuO/CeO2/ZrO2 has better low-temperature redox property, larger CO2 desorption peak area and higher catalytic activity for CO oxidation. |
Keywords: impregnation method CuO-CeO2/ZrO2 catalytic activity CO oxidation |
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杨志强,毛东森,杨超杰,郭强胜,卢冠忠.制备方法对CuO-CeO2/ZrO2催化CO氧化性能的影响[J].无机化学学报,2012,28(7):1353-1359. |
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