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浙江大学学报(理学版)  2017, Vol. 44 Issue (4): 485-492    DOI: 10.3785/j.issn.1008-9497.2017.04.015
化学     
铜掺杂对Fe/β催化剂NH3-SCR催化性能的影响
赵茹, 姜水燕, 周仁贤
浙江大学 化学系 催化研究所, 浙江 杭州 310028
The effect of Cu doping on catalytic performance of Fe/β catalyst for NH3-SCR
ZHAO Ru, JIANG Shuiyan, ZHOU Renxian
Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou 310028, China
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摘要: 制备了一系列Cu掺杂量不同的Fe/β(40)催化剂,并采用ICP-AES、XRD、H2-TPR、UV-vis和XPS等表征技术分析了催化剂的物化性质.结果表明,适量的铜掺杂能大大提高Fe/β(40)催化剂的低温活性,拓宽其活性温度窗口,但过量的Cu掺杂会降低催化剂的N2选择性.Cu掺杂质量比为1.27% Cu-2% Fe/β(40)的催化剂具有最佳的SCR性能,这与催化剂中存在较多离子交换位的Fe3+和Cu2+物种有关,而存在较多的CuO物种会促进氨高温氧化,使催化剂的N2选择性降低且高温窗口变窄.高温水热条件下Cu的存在可能使Cu、Fe物种更容易发生迁移和团聚,导致Cu-Fe/β(40)催化剂的水热稳定性明显变差.
关键词: NH3-SCRCu-Fe/β(40)铜掺杂水热老化    
Abstract: The Cu doped Fe/β (40) catalysts were prepared by ion-exchanged/wetness-impregnation methods and characterized using various analytical techniques, including H2-TPR, XRD, UV-vis and XPS. Appropriate amount of copper enormously improved the low temperature activity of Fe/β (40) and broadened the temperature window of activity. Excessive amount of copper decreased the N2 selectivity of catalysts. 1.27%Cu-2%Fe/β catalyst obtained the best performance attributed to many ion-exchanged positions of Fe3+ and Cu2+. However, a large amount of CuO can promote NH3 oxidation at high temperature, and decrease N2 selectivity and narrow down the temperature window of activity. Cu doping may make the migration and agglomeration of Cu and Fe species more easily under high-temperature hydrothermal conditions, which leads to hydrothermal stability of Cu-Fe/β (40) catalyst change.
Key words: NH3-SCR    Cu-Fe/β(40)    Cu doping    hydrothermal aging
收稿日期: 2016-07-08 出版日期: 2017-12-09
CLC:  O643  
基金资助: 浙江省重点科技创新团队计划资助项目.
通讯作者: 周仁贤,ORCID:http://orcid.org/0000-0002-5627-070X,E-mail:zhourenxian@zju.edu.cn.     E-mail: zhourenxian@zju.edu.cn
作者简介: 赵茹(1990-),ORCID:http://orcid.org/0000-0001-6295-3008,女,硕士研究生,主要从事柴油车尾气脱硝研究,E-mail:21437079@zju.edu.cn.
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引用本文:

赵茹, 姜水燕, 周仁贤. 铜掺杂对Fe/β催化剂NH3-SCR催化性能的影响[J]. 浙江大学学报(理学版), 2017, 44(4): 485-492.

ZHAO Ru, JIANG Shuiyan, ZHOU Renxian. The effect of Cu doping on catalytic performance of Fe/β catalyst for NH3-SCR. Journal of ZheJIang University(Science Edition), 2017, 44(4): 485-492.

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https://www.zjujournals.com/sci/CN/10.3785/j.issn.1008-9497.2017.04.015        https://www.zjujournals.com/sci/CN/Y2017/V44/I4/485

[1] BAIKER A, DOLLENMEIER P, GLINSKI M, et al. Selective catalytic reduction of nitric oxide with ammonia:I. monolayer and multilayers of vanadia supported on titania[J]. Applied Catalysis,1987,35(2):351-364.
[2] BOSCH H, JANSSEN F. Formation and control of nitrogen oxides[J]. Catalysis Today,1988(2):369-379.
[3] BUSCA G, LIETTI L, RAMIS G, et al. Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:A review[J]. Applied Catalysis B:Environmental,1998,18:1-36.
[4] MUTIN P H, POPA A F, VIOUX A, et al. Nonhydrolyticvanadia-titaniaxerogels:Synthesis, cha-racterization, and behavior in the selective catalytic reduction of NO by NH3[J]. Applied Catalysis B:Environmental,2006,69:49-57.
[5] KANG M, YEON T H, PARK E D, et al. Novel MnOx catalysts for NO reduction at low temperature with ammonia[J]. Catalysis Letters,2006,106:77-80.
[6] BALLE P, GEIGER B, KURETI S. Selective catalytic reduction of NOx by NH3 on Fe/HBEA zeolite catalysts in oxygen-rich exhaust[J]. Applied Catalysis B:Environmental,2009,85:109-119.
[7] DJERAD S, CROCOLL M, KURETI S, et al. Effect of oxygen concentration on the NOx reduction with ammonia over V2 O5-WO3/TiO2 catalyst[J]. Catalysis Today,2006,113:208-214.
[8] DUNN J P, KOPPULA P R, STENGER H G, et al. Oxidation of sulfur dioxide to sulfur trioxide over supported vanadia catalysts[J]. Applied Catalysis B:Environmental,1998,19:103-117.
[9] FENG X, HALL W K. FeZSM-5:A durable SCR catalyst for NOx removal from combustion streams[J]. Journal of Catalysis,1997,166:368-376.
[10] LONG R Q, YANG R T. Superior Fe-ZSM-5 catalyst for selective catalytic reduction of nitric oxide by ammonia[J]. Journal of the American Chemical Society,1999,121:5595-5596.
[11] LONG R Q, YANG R T. Catalytic Performance of Fe-ZSM-5 catalysts for selective catalytic reduction of nitric oxide by ammonia[J]. Journal of Catalysis,1999,188:332-339.
[12] SUBBIAH A, CHO B K, BLINT R J, et al. NOx reduction over metal-ion exchanged novel zeolite under lean conditions:Activity and hydrothermal stability[J]. Applied Catalysis B:Environmental,2003,42:155-178.
[13] SJÖVALL H, OLSSON L, FRIDELLE, et al. Selective catalytic reduction of NOx with NH3 over Cu-ZSM-5-The effect of changing the gas composition[J]. Applied Catalysis B:Environmental,2006,64:180-188.
[14] QI G S, YANG R T. Ultra-active Fe/ZSM-5 catalyst for selective catalytic reduction of nitric oxide with ammonia[J]. Applied Catalysis B:Environmental,2005,60:13-22.
[15] JIANG S Y, ZHOU R X. Ce doping effect on performance of the Fe/β catalyst for NOx reduction by NH3[J]. Fuel Process Technol,2015,133:220-226.
[16] TWIGG M V. Catalytic control of emissions from cars[J]. Catalysis Today,2011,163:33-41.
[17] PLÁT F, BÁRTOVÁ S, ŠTěPÁNEK J, et al. Dynamics of a combined DOC-NSRC-SCR exhaust gas after treatment system with periodic regenerations[J]. Industrial & Engineering Chemistry Research,2010,49:10348-10357.
[18] PEREDA-AYO B, DE LA TORRE U, ILLÁN-GÓMEZ M J, et al. Role of the different copper species on the activity of Cu/zeolite catalysts for SCR of NOx with NH3[J]. Applied Catalysis B:Environmental,2014,147:420-428.
[19] ZHANG T, LIU J, WANG D, et al. Selective catalytic reduction of NO with NH3 over HZSM-5-supported Fe-Cu nanocomposite catalysts:The Fe-Cu bimetallic effect[J]. Applied Catalysis B:Environmental,2014,148/149:520-531.
[20] FRANCO R M, MOLINER M, CONCEPCION P, et al. Selective catalytic reduction of NO with NH3 over HZSM-5-supported Fe-Cu nanocomposite catalysts:The Fe-Cu
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