摘要
以H-MOR、H-ZSM-5和H-Beta H型分子筛为载体,采用浸渍法制备了3种铜基分子筛催化剂,利用X射线衍射(XRD)、比表面积分布测试(BET)、NH_(3)程序升温脱附(NH_(3)-TPD)、H_(2)程序升温还原(H_(2)-TPR)、X射线荧光光谱(XRF)和X射线光电子能谱(XPS)等表征手段对该催化剂的物化特性进行分析,并对其在200~650℃范围内的NH_(3)-SCR脱硝性能进行评价。结果表明:3种铜基分子筛催化剂的活性温度窗口不同,Cu/MOR、Cu/ZSM-5和Cu/Beta催化剂达到80%脱硝效率的活性温度窗口分别位于280~550℃、250~400℃和350~450℃;负载Cu后的分子筛骨架结构基本保持不变;相比H型分子筛催化剂,Cu/Beta和Cu/ZSM-5催化剂的比表面积增加,Cu/MOR催化剂的比表面积和孔体积却有所下降;Cu/MOR和Cu/ZSM-5催化剂表现出较好的氧化还原能力,且其表面具有更多的CuO物种和表面吸附氧(Oα)含量;NH_(3)-TPD结果显示,Cu的引入使Beta和ZSM-5分子筛表面的强酸量减弱,MOR分子筛的强酸量增加,使Cu/MOR催化剂高温段NH_(3)-SCR反应中的NH_(3)吸附增强,从而表现出较为优异的高温催化活性。
Three Cu-based zeolite catalysts were prepared by the impregnation method using H-MOR,H-ZSM-5,and H-Beta as carriers,the physical and chemical properties o£the catalysts were characterized by X-ray diffraction(XRD),brunauer-emmett-teller(BET),temperature-programmed desorption of ammonia(NH3-TPD),temperature programmed reduction of hydrogen(H_(2)-TPR),X ray fluorescence spectroscopy(XRF)and X-ray photoelectron spectroscopy(XPS),and the ammonia selective catalytic reduction(NH_(3)-SCR)reaction performance in the range of 200-650℃ was evaluated.The results show the active temperature windows o£the three copper-based zeolite catalysts are quite different,and the temperature windows for the denitration efficiency above 80%of Cu/MOR,Cu/ZSM-5,and Cu/Beta are respectively 280-550℃,250-400℃,and 350-450℃.The framework structure of the catalyst molecular sieves after Cu loading remained basically unchanged.Compared with the H-type zeolite catalysts,the specific surface area of Cu/Beta and Cu/ZSM-5 increased,while the specific surface area and pore volume of Cu/MOR decreased.Cu/MOR and Cu/ZSM-5 showed better redox ability,and also had more CuO and surface adsorbed oxygen(Oa)content.The NH_(3)-TPD results showed that the introduction of Cu weakened the amount of strong acid on the surface of Beta and ZSM-5,while the amount o£strong acid on the surface of Cu/MOR increased,which enhanced the NH3 adsorption in the high-temperature NH3-SCR reaction,thus showing relatively excellent high-temperature catalysis performance.
作者
靳鹏凯
陈志勇
金瑞奔
陈阳
刘志坦
庄柯
喻乐蒙
盛重义
JIN Pengkai;CHEN Zhiyong;JIN Ruiben;CHEN Yang;LIU Zhitan;ZHUANG Ke;YU Lemeng;SHENG Zhongyi(School of Environment 9Nanjing Normal University,Nanjing 210023,China;Yining Heat Supply Co,,Ltd.,Yining 835008,China;Hangzhou Tianliang Detection Technology Co.,Ltd.,Hangzhou 312012,China;National Energy Group Science and Technology Research Institute Co.,Ltd.,Nanjing 210023,China;Guodian EnvironmentaI Protection Research Institute Co,,Ltd.,Nanjing 210031,China;College of Chemistry&Environmental Sciences,Yili Normal University,Yining 835012,CA£na)
出处
《安全与环境工程》
CAS
CSCD
北大核心
2023年第2期233-240,共8页
Safety and Environmental Engineering
基金
国家自然科学基金项目(41877469)
江苏省社会发展面上项目(BE2020754)
国家环境保护大气物理模拟与污染控制重点实验室开放基金项目(D2020Y004)。
