| 李惠娟,蒋晓原,郑小明.介质阻挡放电等离子体辅助CuO/CeO2-TiO2/r-Al2O3[J].分子催化,2014,(2):157-164 |
| 介质阻挡放电等离子体辅助CuO/CeO2-TiO2/r-Al2O3 |
| Non-thermal-plasma combined with selective catalytic reaction of NO by CH4 over CuO/CeO2/TiO2 /?r-Al2O3 catalyst |
| 投稿时间：2013-12-09 修订日期：2014-01-28 |
| DOI： |
| 中文关键词: 等离子体 氧化铜 氧化铈 NO+CH4 NO+CH4+O2 |
| 英文关键词:plasma, CuO, CeO2, NO+CH4 , NO+CH4+O2 |
| 基金项目: |
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| 摘要点击次数: 1924 |
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| 中文摘要: |
| 摘要：在介质阻挡等离子体放电（DBD）辅助催化剂 (6%CuO/15%TiO2/-Al2O3，6%CuO/5%CeO2/15%TiO2/-Al2O3)反应装置上，研究了4种不同反应条件下（NO+CH4, NO+CH4+O2, NO+CH4+NTP, NO+CH4+O2+NTP）NO和CH4反应，采用BET、XRD、H2-TPR和XPS等手段对催化剂进行了表征。结果表明在上述4种反应条件下，对于NO+CH4的反应，O2的存在有利于NO脱除，在等离子体条件下，O2的加入对NO的转化有所抑制；而等离子体的活化极大增强了NO的低温脱除活性。在等离子体存在条件下，6%CuO/5%CeO2/15%TiO2/-Al2O3(6Cu5Ce15TA) 对NO的转化率都优于6%CuO/15%TiO2/-Al2O3（6Cu15TA）。BET结果显示添加TiO2和CeO2于-Al2O3表面后，比表面积都有少量降低；而各载体负载6%CuO后比表面积也有所下降。XRD结果表明6Cu15TA和6Cu5Ce15TA催化剂由锐钛矿相TiO2组成，CuO在各催化剂表面呈现高度分散。H2-TPR数据和XPS实验结果显示负载CuO后，催化剂表面的铜物种由高度分散的CuO和嵌入到CeO2或TiO2晶格中Cu2+所组成。6Cu5Ce15TA表面含有较6Cu15TA多的Cu+，从而增强了NO的脱除活性。 |
| 英文摘要: |
| Abstract: NOx emissions from utility boilers and diesel engines are the leading contributors to acid rain as well as to the photochemical smog through the formation of ozone. TiO2/γ-Al2O3 binary system was regarded as a very promising support for DENOx catalysts and in many other potential applications. Cerium dioxide (CeO2) was very important for some catalytic applications. The Cu-based catalysts were widely used for NO removal. In our experiment, 6%CuO/TiO2--Al2O3 and 6%CuO/5%CeO2/TiO2--Al2O3 on NO+CH4 reaction were investigated under plasma-assisted systems with or without oxygen. The catalysts were characterized by BET, XRD, H2-TPR and XPS methods. The results showed that the catalytic activities of CuO/CeO2/TiO2--Al2O3 were superior to CuO/TiO2--Al2O3 except for NO+CH4 reactions, and NO conversions reached 100% at 300℃ and 350℃ for NO+CH4 reaction with plasma, respectively. BET and XRD characterization showed that -Al2O3 had the largest specific surface area, which decreased after TiO2, CeO2 and CuO loading on. Weak CuO crystalline diffraction peaks could find on 6Cu15TA and CeO2 crystalline diffraction peaks on 6Cu5Ce15TA. H2-TPR results showed that the three reduction peaks belong to highly dispersed CuO, -Cu-O-Ti-O- and CeO2 for the two catalysts. And XPS suggested that the surface of 6Cu5Ce15TA had more Cu+ species than 6Cu15TA, which resulted in more catalytic activity for NO removal. |
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