• 关键词：二氧化硫  Cu-Ce-O  催化剂  碳烟氧化  硫酸盐

• 基金项目：广东省社会发展科技项目(No.2007B030102006);广州市属高校科技项目(No.62008)

• 陈瑜
• 华南理工大学环境科学与工程学院, 广州 510006

• 叶代启
• 华南理工大学环境科学与工程学院, 广州 510006

• 付名利
• 华南理工大学环境科学与工程学院, 广州 510006

• 梁红
• 广州大学化学化工学院, 广州 510006

• 摘要：运用程序升温氧化(TPO)对共沉淀法合成的Cu-Ce-O催化剂进行了活性评价,考察了在不同浓度的SO₂气氛下Cu-Ce-O催化剂氧化模拟碳黑的性能,并用BET、XRD、TPR和FT-IR对催化剂进行了表征.BET和XRD测试显示,Cu和Ce的结合使催化剂比表面积增大,晶体结构发生变化,形成了复合氧化物;TPO活性测试结果表明,Cu-Ce-O复合催化剂比单一组分的CuO或CeO₂具有更好的低温催化活性.复合氧化物Cu-Ce-O中Cu原子含量越高,对应硫化后的催化剂氧化碳烟的能力越低,同时催化剂表面生成的硫酸盐越多,即催化剂抗硫中毒能力也降低.浓度低于0.03%的SO₂对Cu-Ce-O的催化性能有一定的促进作用,但SO₂的体积分数超过0.03%后碳黑燃烧速率变慢;FT-IR初步证实了高体积分数的SO₂所产生的大量SO₄^2-可能是抑制催化剂活性的原因.

• Abstract：Cu-Ce-O catalysts were prepared by co-precipitation and their catalytic behavior was investigated by Temperature Programmed Oxidation (TPO) for model soot oxidation in a feed gas containing various concentrations of SO₂.The catalysts were characterized by BET,XRD,TPR and FT-IR.The BET and XRD results showed that the combination of Cu and Ce oxides increased their specific surface area,changed the crystal structure and formed complex oxides.TPO tests revealed that Cu-Ce-O complexes exhibited better activity than pure CuO or CeO₂ at lower temperatures.An increase in the Cu atomic ratio in sulfated Cu-Ce-O was accompanied by a simultaneous increase of the combustion temperature and the amount of surface sulfate,which could imply the deterioration of sulfur tolerance of those catalysts.SO₂ with concentration below 0.03% enhanced the catalytic performance of Cu-Ce-O,but the soot oxidation rate began to slow down at SO₂ feed concentrations above 0.03%.The FT-IR spectrum revealed that the introduction of high concentrations of SO₂ produced plentiful SO₂-4 on the catalyst surface,which could account for the loss of activity of the Cu-Ce-O catalysts.

• Key words：sulfur dioxide  Cu-Ce-O  catalyst  soot oxidation  sulfate

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