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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

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李瑞睿, 孔祥成, 王晓, 张娜娜, 辛颖, 李倩, 张昭良. Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能[J]. 环境化学, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
引用本文: 李瑞睿, 孔祥成, 王晓, 张娜娜, 辛颖, 李倩, 张昭良. Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能[J]. 环境化学, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
shu
LI Ruirui, KONG Xiangcheng, WANG Xiao, ZHANG Nana, XIN Ying, LI Qian, ZHANG Zhaoliang. Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3[J]. Environmental Chemistry, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
Citation: LI Ruirui, KONG Xiangcheng, WANG Xiao, ZHANG Nana, XIN Ying, LI Qian, ZHANG Zhaoliang. Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3[J]. Environmental Chemistry, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
shu

Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能

  • 1.

    济南大学, 化学化工学院, 济南, 250022;

  • 2.

    济宁市环境保护监测站, 济宁, 272000

  • 基金项目:

    国家自然科学基金（21477046）和山东省重点研发计划（重大关键技术）（2016ZDJS11A03）资助.

Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3

  • 1.

    School of Chemistry and Chemical Engineering, University of Ji'nan, Ji'nan, 250022, China;

  • 2.

    Jining Environmental Protection Monitoring Station, Jining, 272000, China

  • Fund Project: Supported by the National Natural Science Foundation of China (21477046) and Key Technology R&D Program of Shandong Province (2016ZDJS11A03).

  • 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 NOx with NH3 (NH3-SCR) is regarded as one of the primary technologies for deNOx in 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,inductively coupled 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% NOx conversion 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.
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  • 收稿日期:  2018-01-11
  • 刊出日期:  2018-06-15
李瑞睿, 孔祥成, 王晓, 张娜娜, 辛颖, 李倩, 张昭良. Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能[J]. 环境化学, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
引用本文: 李瑞睿, 孔祥成, 王晓, 张娜娜, 辛颖, 李倩, 张昭良. Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能[J]. 环境化学, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
shu
LI Ruirui, KONG Xiangcheng, WANG Xiao, ZHANG Nana, XIN Ying, LI Qian, ZHANG Zhaoliang. Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3[J]. Environmental Chemistry, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
Citation: LI Ruirui, KONG Xiangcheng, WANG Xiao, ZHANG Nana, XIN Ying, LI Qian, ZHANG Zhaoliang. Preparation and performance of Cu-SAPO-44 for selective catalytic reduction of NOx with NH3[J]. Environmental Chemistry, 2018, 37(6): 1264-1271. doi: 10.7524/j.issn.0254-6108.2018011001
shu

Cu-SAPO-44的制备及氨选择性催化还原氮氧化物的性能

  • 1.  济南大学, 化学化工学院, 济南, 250022;
  • 2.  济宁市环境保护监测站, 济宁, 272000
  • 收稿日期:  2018-01-11
基金项目:

国家自然科学基金（21477046）和山东省重点研发计划（重大关键技术）（2016ZDJS11A03）资助.

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.

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