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化工学报  2015 

气凝胶骨架镶嵌的CeO2纳米团簇催化氧化HCl制Cl2

DOI: 10.11949/j.issn.0438-1157.20150902, PP. 3421-3427

Keywords: 氧化铈,纳米团簇,气凝胶,氯循环,催化氧化,动力学

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Abstract:

采用一步溶胶-凝胶法制备了镶嵌于气凝胶骨架内的CeO2纳米团簇催化材料(CeO2@MxOy,MxOy=SiO2、ZrO2、Al2O3)用于HCl催化氧化反应。镶嵌于气凝胶骨架内的CeO2纳米团簇显著的量子尺寸效应导致其表现出不同于晶相CeO2的特性,H2-TPR测试结果显示在晶相CeO2表面氧物种还原温区内CeO2纳米团簇即可被充分还原。优异的氧化还原性能导致CeO2@MxOy在HCl氧化过程具有良好的催化活性,其中,40CeO2@SiO2的活性最高,在接触时间为0.1598h,VO2/VHCl为1,430℃时,Cl2空时产率可以达到2.10g·(gcat)-1·h-1。催化剂表面的HCl氧化反应同时受O2分压和HCl分压的影响,这表明Cl2从催化剂表面的脱附是该反应的决速步骤。

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