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Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能
Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3
【摘要】 氨选择性催化还原(NH3-SCR)是消除柴油车尾气NOx的主要技术,Cu-微孔分子筛催化剂展现了优异的活性和稳定性.本文采用直接离子交换法(DIE)和传统离子交换法(CIE)分别制备了Cu-SAPO-44催化剂.X射线粉末衍射(XRD)表征发现,在CIE过程中,硝酸铵的交换导致了SAPO-44结晶度下降,因此,CIE样品的比表面积降低.氨气程序升温脱附(NH3-TPD)表明,DIE样品比CIE样品拥有更多的酸性位和较强的NH3吸附能力.同时,氢气程序升温还原(H2-TPR)表明,DIE样品更容易发生氧化还原反应.然而,电感耦合等离子体发射光谱仪(ICP-AES)测得的Cu含量,DIE样品远低于CIE样品.对比两者的脱硝活性,发现铜含量较低的DIE样品和铜含量较高的CIE样品在250℃均可达到98%的NOx转化率和接近100%的N2选择性.动力学结果表明,DIE样品的本征活性(转换频率)略高于CIE样品.由此,Cu-SAPO-44催化剂在NH3-SCR领域具有潜在的广阔应用前景.
【Abstract】 Selective catalytic reduction of NOxwith NH3(NH3-SCR) is regarded as one of the primary technologies for de NOxin diesel exhaust.Cu-based microporous zeolites are widely used in NH3-SCR due to their its excellent SCR activity and high thermal stability.In this paper,Cu-SAPO-44 zeolites were synthesized by direct ion-exchange(DIE) and conventional ion-exchange(CIE)methods.X-ray powder diffraction(XRD) results indicate that the DIE sample experienced a significant drop in crystallinity during the ion-exchange stage of ammonia nitrate.Therefore,the specific surface area of the CIE sample decreased.Temperature-programmed desorption of NH3(NH3-TPD) showed that the DIE sample possesseed more acid sites and higher NH3 adsorption capacity compared with the CIE sample.Simultaneously,temperature-programmed reduction with H2(H2-TPR) illustrated that the DIE sample exhibited better redox ability.However,inductivelycoupled plasma-atomic emission spectromety(ICP-AES) revealed that the DIE sample had much lower Cu loading in comparison with the CIE sample.Interestingly,both the DIE and CIE samples achieve 98% NOxconversion and approximately 100% N2 selectivity at 250 ℃.The kinetics study demonstrated that the intrinsic activity(TOF) of the DIE sample was slightly higher than that of the CIE sample.Thereby,the Cu-SAPO-44 catalyst has a great potential in the NH3-SCR field.
- 【文献出处】 环境化学 ,Environmental Chemistry , 编辑部邮箱 ,2018年06期
- 【分类号】O643.3;X734.2
- 【被引频次】1
- 【下载频次】163