Fe改性Cu-SSZ-13的方法对催化剂NH3-SCR脱硝性能的影响

doi:10.16085/j.issn.1000-6613.2016.12.024

化工进展 ›› 2016, Vol. 35 ›› Issue (12): 3898-3906.DOI: 10.16085/j.issn.1000-6613.2016.12.024

Fe改性Cu-SSZ-13的方法对催化剂NH₃-SCR脱硝性能的影响

赵文雅^1,2,3, 李永红^1,2,3, 刘小娇^1,2,3, 张冉冉^1,2,3

1 天津大学化工学院绿色合成与转化教育部重点实验室, 天津 300072;
2 精馏技术国家工程研究中心, 天津 300072;
3 天津化学化工协同创新中心, 天津 300072

收稿日期:2016-03-28 修回日期:2016-05-12 出版日期:2016-12-05 发布日期:2016-12-05
通讯作者: 李永红,教授,博士生导师。E-mail:yhli@tju.edu.cn。
作者简介:赵文雅(1989-),女,硕士研究生。

Effect of preparation methods on de-NO_x performance of Fe/Cu-SSZ-13 catalyst for NH₃-SCR

ZHAO Wenya^1,2,3, LI Yonghong^1,2,3, LIU Xiaojiao^1,2,3, ZHANG Ranran^1,2,3

1 Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, China;
2 National Engineering Research Center for Distillation Technology, Tianjin 300072, China;
3 Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China

Received:2016-03-28 Revised:2016-05-12 Online:2016-12-05 Published:2016-12-05

摘要/Abstract

摘要： 为了解决柴油车尾气中的NO_x污染环境的问题，分别用离子交换法（IE）、湿浸渍法（IWI）和固态离子交换法（SSIE）制备了3种Fe/Cu-SSZ-13分子筛催化剂，考察了其对NH₃选择性催化还原NO（NH₃-SCR）的催化性能，并运用XRD、BET、FTIR、UV-Vis DRS，H₂-TPR等方法对催化剂进行了表征。结果表明，经Fe改性Cu-SSZ-13后，催化剂有很好的抗高空速性能、较宽的温度窗口、很好的水热稳定性和更好的高温还原能力。制备方法对Fe/Cu-SSZ-13的脱硝活性影响不同，在150～400℃温度范围时，3种催化剂的SCR活性顺序为：Fe（5.5%）-IE >Fe（5.4%）-SSIE >Fe（5.5%）-IWI；然而高于400℃时，SCR活性顺序为：Fe（5.5%）-IE >Fe（5.5%）-IWI >Fe（5.4%）-SSIE。表征结果显示，3种方法制备的催化剂进行比较，离子交换法制备的Fe含量为5.5%的催化剂表现出最好的水热稳定性、最大的比表面积以及最好的催化活性，其在175～500℃内NO的转化率达到90%以上，因此Fe（5.5%）-IE是首选的NH₃-SCR催化剂。

关键词: 分子筛, 催化剂, 选择催化还原, 活性, SSZ-13, 分子筛改性

Abstract: To solve the environmental problem of NO_x in diesel exhaust,a series of Fe/Cu-SSZ-13 molecular sieves catalysts were prepared by liquid ion exchange(IE),incipient wet-impregnation (IWI) and solid-state ion exchange(SSIE)methods respectively. The catalytic performances for selective catalytic reduction (NH₃-SCR) were examined and the catalysts were characterized using XRD,BET,FTIR,UV-Vis DRS,H₂-TPR. The characterization results indicated that the catalysts could be used under a high space velocity,and had wider temperature range,prefect hydrothermal stability,and better high temperature SCR ability. The denitration activity of Fe/Cu-SSZ-13 catalysts was affected by their preparation method. From 150℃ to 400℃,the activity order of the SCR catalysts was:Fe(5.5%)-IE >Fe(5.4%)-SSIE >Fe(5.5%)-IWI. However,above 400℃,the activity order became:Fe(5.5%)-IE >Fe(5.5%)-IWI >Fe(5.4%)-SSIE. Moreover,the catalyst prepared by IE,with Fe concentration of 5.5%,showed the best hydrothermal stability,the largest specific surface area and the best catalytic activity,with NO conversion over 90% from 175℃ to 500℃,So Fe(5.5%)-IE was the best NH₃-SCR catalysts.

Key words: molecular sieves, catalyst, selective catalytic reduction(SCR), reactivity, SSZ-13, modification of zeolite

中图分类号:

TQ032

赵文雅, 李永红, 刘小娇, 张冉冉. Fe改性Cu-SSZ-13的方法对催化剂NH₃-SCR脱硝性能的影响[J]. 化工进展, 2016, 35(12): 3898-3906.

ZHAO Wenya, LI Yonghong, LIU Xiaojiao, ZHANG Ranran. Effect of preparation methods on de-NO_x performance of Fe/Cu-SSZ-13 catalyst for NH₃-SCR[J]. Chemical Industry and Engineering Progree, 2016, 35(12): 3898-3906.

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Fe改性Cu-SSZ-13的方法对催化剂NH₃-SCR脱硝性能的影响

Effect of preparation methods on de-NO_x performance of Fe/Cu-SSZ-13 catalyst for NH₃-SCR

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