催化剂Cu/HZSM-5的硅铝比对催化分解N2O的影响  

Effect of silica-alumina ration of Cu/HZSM-5 catalyst on N2O catalytic decomposition

作　　者：徐庆生 宋永吉 刘久欣 王新承 李翠清 王虹 XU Qingsheng;SONG Yongji;LIU Jiuxin;WANG Xincheng;LI Cuiqing;WANG Hong(Bejing Key Laboratory of Fuels Cleaning and Advanced Catalytic Enmission Reduction Technology,College of Chemical Engineering,Beiing Institute of Petrochemical Technology,Bejing 102617,China;Collee of Environment and Energy Engineering,Beijing University of Technology,Beijig 100124,China)

机构地区：[1]北京石油化工学院化学工程学院,燃料清洁化及高效催化减排技术北京市重点实验室,北京102617 [2]北京工业大学环境与能源工程学院,北京100124

出　　处：《环境工程学报》2020年第6期1579-1591,共13页Chinese Journal of Environmental Engineering

基　　金：国家自然科学基金资助项目(20176012,21076025)。

摘　　要：为系统研究Cu/HZSM-5硅铝比对其各类性能的影响,采用等体积浸渍法与离子交换法,以硅铝比为27、50、117的HZSM-5为载体,制备负载型N2O催化分解催化剂Cu/HZSM-5和Cu/ZSM-5,催化剂的活性组分为CuO。通过催化剂反应活性评价、X射线荧光光谱分析、X射线衍射分析结果,对2种方法制备催化剂活性的差异进行了分析。利用比表面积孔径分析仪(BET)、X射线衍射分析(XRD)、场发射扫描电镜(SEM)、X射线荧光光谱分析(XRF)、氢气程序升温还原分析(H2-TPR)、氨气程序升温脱附分析(NH3-TPD)等表征手段对催化剂物化性质等进行分析,得到载体HZSM-5的硅铝比差异对催化剂特征结构、比表面积、特征形貌、酸性位数量、可还原性能的影响规律。等体积浸渍法制备的催化剂活性评价结果表明,硅铝比为27的Cu8/HZSM-5催化剂活性最好,完全催化分解N2O的温度在400℃左右。水热稳定性实验结果以及寿命实验结果表明,硅铝比为27的Cu8/HZSM-5具有良好的水热稳性,3种硅铝比的Cu8/HZSM-5催化剂均具备良好的热稳定性。Cu/HZSM-5的活性评价以及各种表征结果显示,在一定范围内,硅铝比越低,催化剂活性越好。In order to systematically study the effect of silica-alumina ratio on various properties of Cu/HZSM-5,two catalysts of Cu/HZSM-5 and Cu/ZSM-5, being supported on HZSM-5 with the silica to alumina ratios of 27, 50 and 117, for N2O catalytic decomposition were prepared by incipient wetness impregnation method and ion exchange method, and the active component was CuO. The difference in catalytic activity among the catalysts prepared by these two methods was compared through catalyst activity evaluation, X-ray fluorescence spectra and X-ray diffraction patterns. The physicochemical properties of the catalysts were characterized by specific surface area pore size analyzer(BET), X-ray diffraction(XRD), field emission scanning electron microscopy(SEM), X-ray fluorescence spectrometry(XRF), hydrogen temperature programmed reduction(H2-TPR), and ammonia temperature programmed desorption(NH3-TPD). The influence of silica-alumina ratio of supporter HZSM-5 on the structure, specific surface area, morphology, the number of acid sites and reducibility of CuO were analyzed. The catalyst reaction activity results showed that Cu8/HZSM-5 catalyst with silicaalumina ratio of 27 presented the best activity, which was prepared by the incipient wetness impregnation method. The temperature of complete catalytic decomposition of N2O was about 400℃. The results of hydrothermal stability and life test experiments revealed that Cu8/HZSM-5 with a silica to alumina ratio of 27 had the optimum hydrothermal stability. All Cu8/HZSM-5 catalysts showed desirable thermal stability. Through the activity evaluation and various characterization results of Cu/HZSM-5, it was shown that in a certain range,the lower the Si-Al ratio is, the better the catalyst activity is. Through the activity evaluation and various characterization results of Cu/HZSM-5, it was shown that in a certain range, the lower the Si-Al ratio is, the better the catalyst activity is.

关 键 词：氧化亚氮 催化分解 催化剂 HZSM-5 硅铝比 Cu物种 

分 类 号：X511[环境科学与工程—环境工程]