不同硅铝比Fe-ZSM-5催化剂对氧化亚氮催化分解性能的研究

以不同硅铝比的H-ZSM-5分子筛为载体,采用离子交换法和化学气相沉积法制备Fe-ZSM-5催化剂,并用XRD、BET、TEM、UV-vis和NH3-TPD等表征手段对催化剂进行分析,研究催化剂中铁的存在状态.结果表明,分子筛的硅铝比影响铁在分子筛中的分布形态,化学气相沉积法和热离子交换法制得硅铝比为25的Fe-ZSM-5-25分子筛催化剂上均匀地分布着粒径为8 nm左右的纳米氧化铁颗粒,并且Fe-ZSM-5-25分子筛催化剂比Fe-ZSM-5-300更容易形成Fe3+x O y团簇.制得的Fe-ZSM-5分子筛催化剂催化分解氧化亚氮(N2O),结果表明,相同的制备方法,硅铝比小的Fe-ZSM-5-25催化剂对N2O分解活性更好;相同硅铝比的Fe-ZSM-5催化剂,采用化学气相沉积法制得的对N2O分解活性最好.另外,O2的存在对Fe-ZSM-5上N2O催化分解活性有抑制作用,而NO对N2O催化分解活性展示了一定的正效应.最后,经过100 h的连续反应,Fe-ZSM-5催化剂依然能够保持催化活性.

Fe-ZSM-5 Catalysts with Different Silica-Alumina Ratios for N2O Catalytic Decomposition

The Fe-ZSM-5 catalysts were prepared with H-ZSM-5 of different Si/Al ratios by wet ion exchange and chemical vapor deposition. Then the catalysts were investigated by XRD, BET, TEM, UV-vis and NH₃-TPD technologies to analyze the iron states in Fe-ZSM-5 zeolites. The results showed that after H-ZSM-5 zeolites were prepared by chemical vapor deposition and heating wet ion exchange, the nano Fe₂O₃ particles were uniformly dispersed with the sizes of 8 nm in the Fe-ZSM-5-25 (Si/Al-25). Moreover, there were more oligonuclear Fe_x³⁺O_y clusters in the Fe-ZSM-5-25 catalysts than in Fe-ZSM-5-300 (Si/Al-300). The results of catalytic performance on N₂O decomposition showed that Fe-ZSM-5-25 catalysts had higher catalytic activities than Fe-ZSM-5-300 catalysts. The Fe-ZSM-5 catalysts prepared by chemical vapor deposition achieved the best catalytic activity in N₂O decomposition among the catalysts prepared by the three methods. Moreover, the presence of O₂ only slightly reduced N₂O conversion, while NO promoted the N₂O decomposition. Finally, after reaction for more than 100 h, Fe-ZSM-5 catalyst showed no obvious deactivation under simulated emission conditions.