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低温等离子体协同Ag/Al₂O₃选择性催化丙烯还原氮氧化物反应的原位红外光谱研究

In Situ DRIFTS Study on Non-thermal Plasma-Assisted NO_x Reduction by Propene over Ag/Al₂O₃ Catalyst

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【Author】 KE Rui~1,LI Junhua~(2*),HAO Jiming~2,FU Lixin~2,CHEN Qiang~1,ZHAO Daqing~1(1 Department of Mechanical Engineering,Tsinghua University,Beijing 100084,China;2 Department of Environmental Science and Engineering,Tsinghua University,Beijing 100084,China)

【机构】清华大学机械工程系；清华大学环境科学与工程系；清华大学机械工程系北京100084；北京100084；北京100084；

【摘要】研究了稀燃条件下低温等离子体(NTP)协同丙烯在Ag/Al2O3催化剂上选择性催化还原NOx反应,通过原位漫反射傅里叶变换红外光谱(DRIFTS)对NTP协同前后反应气中NO和C3H6的吸附以及丙烯选择性催化还原反应进行了表征.结果表明,丙烯的活化是Ag/Al2O3上选择性催化还原反应的关键步骤.NTP活化反应气体后,Ag/Al2O3表面-NCO、R-NO2和有机酸根等物种的数量大幅度增加,并且其催化还原NOx的低温(<350℃)活性也显著提高.在NTP协同前后,选择性催化还原过程可能存在两条反应路径,较低温度下主要是-NCO生成N2,而较高温度下则是-CN向N2转化.更多还原

【Abstract】 The non-thermal plasma（NTP）-assisted selective catalytic reduction（SCR） of NO_x by propene over the Ag/Al₂O₃ catalyst was investigated.In situ diffuse reflectance infrared Fourier transform spectroscopy（DRIFTS） studies were carried out on the NO and C₃H₆ adsorption and SCR reactions over Ag/Al₂O₃ with or without NTP pretreatment.The results showed that the low-temperature activity of C₃H₆-SCR was remarkably enhanced with the assistance of NTP in the presence of excess oxygen.The activation of propene was the key step in C₃H₆-SCR over Ag/Al₂O₃.After the application of NTP,the amount of（NCO,） R-NO₂ and organic acid species over Ag/Al₂O₃ significantly increased,which caused a high catalytic activity at low temperatures（（<350 ℃））.Two reaction paths were proposed in both SCR and NTP-SCR.At low reaction temperatures,（-NCO） was the key intermediate to generate N₂,while it was（-CN） at high reaction temperatures.更多还原