Fe-V/TiO2催化剂NH3选择性催化还原柴油车尾气NOx

黄海凤; 陈一杰; 杨睿; 朱秋莲; 卢晗锋

Fe-V/TiO₂催化剂NH₃选择性催化还原柴油车尾气NO_x

1.
浙江工业大学生物与环境工程学院, 浙江杭州 310014;
2.
浙江工业大学化学工程与材料科学学院, 浙江杭州 310014

基金项目: 国家自然科学基金（21107096）；浙江省重大科技专项（2007C13042）。

详细信息

通讯作者:
卢晗锋，E-mail：luhf@zjut.edu.cn。

中图分类号: X511
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- 被引次数: 0
出版历程
- 收稿日期: 2013-11-14
- 修回日期: 2014-02-24
- 刊出日期: 2014-06-30

Fe-V/TiO₂ catalysts for selective catalytic reduction of NO_x with NH₃ in diesel exhaust

1.
College of Biological and Environmental Engineering, Zhejiang University of Technology, Hangzhou 310014, China;
2.
Institute of Catalytic Reaction Engineering, Zhejiang University of Technology, Hangzhou 310014, China

摘要

摘要: 采用浸渍法制备了一系列不同Fe/V比例的Fe-V/TiO₂催化剂，考察了催化剂在模拟柴油车尾气中催化还原NO_x的催化性能，采用TG、XRD、H₂-TPR、NH₃-TPD和Raman光谱对催化剂进行了表征。结果表明，当Fe引入后，能显著降低V₂O₅在高温下的挥发，减轻了钒系催化剂在移动源的生物毒性危害。其中，Fe/V比为1：1（Fe₁-V₁/TiO₂）的催化剂形成了FeVO₄活性中心，表现出最好的催化活性，在220~420 ℃ NO_x转化率可达到90%以上。此外，Fe₁-V₁/TiO₂催化剂高温热稳定性较好，并且具有较强的抗硫性能。
- 柴油车尾气 /
- SCR /
- Fe-V/TiO₂催化剂 /
- 抗硫性
Abstract: Fe-V/TiO₂ catalysts with different Fe/V molar ratio were prepared by impregnation method. The catalytic activity of selective catalytic reaction (SCR) were evaluated at the simulation of diesel exhaust environment. The samples were characterized by thermogravimetric analysis, X-ray diffraction, H₂ temperature programmed reduction, NH₃ temperature-programmed desorption and Raman spectra. It was found that the addition of Fe could obviously decrease the losing of V₂O₅ at high temperature, which greatly decreased the toxicity of the vanadium-based catalysts in mobile sources. Among the synthesized catalysts, the Fe₁-V₁/TiO₂ showed the highest activity with the NO_x conversion efficiency over 90% between 220 ℃ and 420 ℃ due to formation of FeVO₄ active sites. Moreover, Fe₁-V₁/TiO₂ exhibited excellent thermal stability at high temperature and sulfur resistance.
- diesel exhaust /
- SCR /
- Fe-V/TiO₂ catalysts /
- sulfur resistance

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参考文献(18)

FU M, GE Y, WANG X, TAN J, YU L, LIANG B. NO_x emissions from Euro IV busses with SCR systems associated with urban, suburban and freeway driving patterns[J]. Sci Total Environ, 2013, 452: 222-226.

PE A, UPHADE B S, SMIRNIOTIS P G. TiO₂-supported metal oxide catalysts for low-temperature selective catalytic reduction of NO with NH₃: I. Evaluation and characterization of first row transition metals[J]. J Catal, 2004, 221(2): 421-431.

MA L, CHENG Y S, CAVATAIO G, MCCABE R W, FU L X, LI J H. Characterization of commercial Cu-SSZ-13 and Cu-SAPO-34 catalysts with hydrothermal treatment for NH₃-SCR of NO_x in diesel exhaust[J]. Chem Eng J, 2013, 225: 323-330.

HUANG H F, JIN L L, LU H F, YU H, CHEN Y J. Monolithic Cr-V/TiO₂/cordierite catalysts prepared by in-situ precipitation and impregnation for low-temperature NH₃-SCR reactions[J]. Catal Commun, 2013, 34: 1-4.

BUSCA G, LUCA L, RAMIS G, BERTI F. Chemical and mechanistic aspects of the selective catalytic reduction of NO_x by ammonia over oxide catalysts: A review[J]. Appl Catal B: Environ, 1998, 18(1/2): 1-36.

LIU F D, SHAN W P, SHI X Y, ZHANG C B, HE H. Research progress in vanadium-free catalysts for the selective catalytic reduction of NO with NH₃[J]. Chin J Catal, 2011, 32(7): 1113-1128.

APOSTOLESCU N, GEIGER B, HIZBULLAH K, JAN M, KURETI S, REICHERT D, SCHOTT F, WEISWEILER W. Selective catalytic reduction of nitrogen oxides by ammonia on iron oxide catalysts[J]. Appl Catal B: Environ, 2006, 62(1/2): 104-114.

BRANDENBERGER S, KR CHER O, TISSLER A, ALTHOFF R. The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH₃[J]. Appl Catal B: Environ, 2010, 95(3/4): 348-357.

MORTON C D, SLIPPER I J, THOMAS M J K, ALEXANDER B D. Synthesis and characterisation of Fe-V-O thin film photoanodes[J]. J Photochem Photobiol A, 2010, 216(2/3): 209-214.

LIU F D, HE H, LIAN Z H, SHAN W P, XIE L J ASAKURA K, YANG W W, DENG H. Highly dispersed iron vanadate catalyst supported on TiO₂ for the selective catalytic reduction of NO_x with NH₃[J]. J Catal, 2013, 307: 340-351.

黄海凤, 金丽丽, 张宏华, 俞河, 卢晗锋. 高抗硫性的铜钒钛低温SCR 脱硝催化剂的制备表征及催化活性[J]. 高校化学工程学报, 2013, 27(4): 722-728. (HUANG Hai-feng, JIN Li-li, ZHANG Hong-hua, YU He, LU Han-feng. Preparation and Characterization of Cu-V/TiO₂ catalysts with strong resistance to SO₂ for low-temperature SCR of NO_x[J]. Journal of Chemical Engineering of Chinese Universities, 2013, 27(4): 722-728.)

MARTIN J, AVILA P, SUAREZ S, YATES M, MARTINROJO A, BARTHELEMY C, MARTIN J. Influence of support acid pretreatment on the behaviour of CoO_x/γ-alumina monolithic catalysts in the CH₄-SCR reaction[J]. Appl Catal B: Environ, 2006, 67(3/4): 270-278.

ETTIREDDY P R, ETTIREDDY N, MAMEDOV S, BOOLCHAND P, SMIRNIOTIS P G. Surface characterization studies of TiO₂ supported manganese oxide catalysts for low temperature SCR of NO with NH₃[J]. Appl Catal B: Environ, 2007, 76(1/2): 123-134.

UDDIN M A, SHIMIZU K, ISHIBE K, SASAOKA E. Characteristics of the low temperature SCR of NO_x with NH₃ over TiO₂[J]. J Mol Catal A: Chem, 2009, 309(1/2): 178-183.

POIZOT P, LARUELLE S, TOUBOUL M, TARASCON J. Wet-chemical synthesis of various iron(Ⅲ) vanadates(V) by co-precipitation route[J]. Comptes Rendus Chimie, 2003, 6(1): 125-134.

H GGBLAD R, MASSA M, ANDERSSON A. Stability and performance of supported Fe-V-oxide catalysts in methanol oxidation[J]. J Catal, 2009, 266(2): 218-227.

LIU Q Y, LIU Z Y, LI C Y. Adsorption and activation of NH₃ during selective catalytic reduction of NO by NH₃[J]. Chin J Catal, 2006, 27(7): 636-646.

SI Z C, WENG D, WU X D, LI J, LI G. Structure, acidity and activity of CuO_x/WO_x-ZrO₂ catalyst for selective catalytic reduction of NO by NH₃[J]. J Catal, 2010, 271(1): 43-51.

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