Cu、Mn、Ce改性V2O5-WO3/TiO2/堇青石催化剂Urea-SCR脱除NO

董国君; 罗璇; 杨治; 梁涛; 张文平

Cu、Mn、Ce改性V₂O₅-WO₃/TiO₂/堇青石催化剂Urea-SCR脱除NO

1.
哈尔滨工程大学材料科学与化学工程学院, 黑龙江哈尔滨 150001;
2.
哈尔滨工程大学动力与能源工程学院, 黑龙江哈尔滨 150001

基金项目: 黑龙江省博士后基金(LRB07-233)。

详细信息

通讯作者:
董国君, 教授, Tel: 13945691027, E-mail: dgj1129@163.com。

中图分类号: O643.3
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- 文章访问数: 1492
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- 被引次数: 0
出版历程
- 收稿日期: 2011-06-13
- 修回日期: 2011-09-26
- 刊出日期: 2012-05-31

Urea-SCR of NO over V₂O₅-WO₃/TiO₂/cordierite catalyst modified with Cu, Mn, Ce

1.
College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China;
2.
College of Power and Energy Engineering, Harbin Engineering University, Harbin 150001, China

Funds: 黑龙江省博士后基金(LRB07-233)。

摘要

摘要: 采用硅胶为黏结剂,在堇青石蜂窝陶瓷上以涂覆法依次负载Cu、Mn、Ce改性的纳米TiO₂粉末、W改性的V₂O₅粉末得到复合催化剂,在120～550 ℃用尿素选择性催化还原(Urea-SCR)氮氧化物时显示良好活性。与商业催化剂V₂O₅-WO₃/TiO₂相比,添加Cu、Mn、Ce后,催化剂脱硝活性显著提高,活性温度窗口明显拓宽。结果表明,催化剂的高活性与催化剂表面适度的酸碱性、高比值的V⁴⁺/V⁵⁺以及良好的氧化还原性能和锐钛矿相的TiO₂、丰富的表面裂纹的存在等因素有关。
- Urea-SCR /
- 氮氧化物 /
- V₂O₅-WO₃/TiO₂ /
- 整体催化剂
Abstract: The cordierite honeycomb ceramics (CC) was coated with Mn, Cu, Ce modified TiO₂, and W modified V₂O₅ in sequence by coating method. A series of monolith catalysts were evaluated at 120～550 ℃ for the selective catalytic reduction (SCR) of NO by urea. Compared to commercial catalyst V₂O₅-WO₃/TiO₂, the SCR performance was significantly improved between a wide temperature with the introduction of Mn, Cu, Ce. The results of characterization suggested that the activity improvement may be contributed to the suitable acidity and basicity of catalyst surface, the high ratio of V⁴⁺/V⁵⁺, the existence of anatase phase TiO₂ and the good redox capability of complex catalyst. This study provides a potential catalyst system for the removal of NO_x from diesel engines.
- Urea-SCR /
- nitrogen oxides /
- V₂O₅-WO₃/TiO₂ /
- monolithic catalyst

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参考文献(25)

TWIGG M V. Progress and future challenges in controlling automotive exhaust gas emissions[J]. Appl Catal B, 2007, 70(1/4): 2-15.

KRCHER O, ELSENER M. Chemical deactivation of V₂O₅/WO₃-TiO₂ SCR catalysts by additives and impurities from fuels, lubrication oils, and urea solution[J]. Appl Catal B, 2008, 77(3/4): 215-227.

VARGAS M A L, CASANOVA M, TROVARELLI A, BUSCA G. An IR study of thermally stable V₂O₅-WO₃-TiO₂ SCR catalysts modied with silica and rare-earths (Ce, Tb, Er)[J]. Appl Catal B, 2007, 75(3/4): 303-311.

PEA D 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.

BRER S, HAMMER T. Selective catalytic reduction of nitrogen oxides by combining a non-thermal plasma and a V₂O₅-WO₃/TiO₂ catalyst[J]. Appl Catal B, 2000, 28(2): 101-111.

WU Z, JIN R, WANG H, LIU Y. Effect of ceria doping on SO₂ resistance of Mn/TiO₂ for selective catalytic reduction of NO with NH₃ at low temperature[J]. Catal Commun, 2009, 10(6): 935-939.

JIANG B, LIU Y, WU Z. Low-temperature selective catalytic reduction of NO on MnO_x/TiO₂ prepared by different methods[J]. J Hazard Mater, 2009, 162(2/3): 1249-1254.

LIN T, ZHANG Q L, LI W, GONG M C, XING Y X, CHEN Y Q. Monolith manganese-based catalyst supported on ZrO₂-TiO₂ for NH₃-SCR reaction at low temperature[J]. Acta Physico-Chimica Sinica, 2008, 24(7): 1127-1131.

WU Z, JIANG B, LIU Y, ZHAO W, GUAN B. Experimental study on a low-temperature SCR catalyst based on MnOx/TiO₂ prepared by sol-gel method[J]. J Hazard Mater, 2007, 145(3): 488-494.

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, 2007, 76(1/2): 123-134.

TANG X, HAO J, YI H, LI J. Low-temperature SCR of NO with NH₃ over AC/C supported manganese-based monolithic catalysts[J]. Catal Today, 2007, 126(3/4): 406-411.

SMIRNIOTIS P G, SREEKANTH P M, PEA D A, JENKINS R G. Manganese oxide catalysts supported on TiO₂, Al₂O₃, and SiO₂: A comparison for low-temperature SCR of NO with NH₃[J]. Ind Eng Chem Res, 2006, 45(19): 6436-6443.

HUANG Y, TONG Z-Q, WU B, ZHANG J-F. Low temperature selective catalytic reduction of NO by ammonia over V₂O₅-CeO₂/TiO₂[J]. J Fuel Chem Technol, 2008, 36(5): 616-620.

SUNG M H, CHOI I S, KIM J S, KIM W S. Agglomeration of yttrium oxalate particles produced by reaction precipitation in semi-batch reactor[J]. Chem Eng Sci, 2000, 55(12): 2173-2184.

唐晓龙, 郝吉明, 易红宏, 宁平, 李俊华. 活性炭改性整体催化剂上低温选择性还原NO_x[J]. 中国环境科学, 2007, 27(6): 845-850. (TANG Xiao-long, HAO Ji-ming, YI Hong-hong, NING Ping, LI Jun-hua. Selective catalytic reduction of NO_x with NH₃ by monolithic catalyst MnO_x/AC/C under low temperature in the presence of excess O₂[J]. China Environmental Science, 2007, 27(6): 845-850.)

ZHOU C-Q, DONG G-J, GONG F, CHANG X. Preparation and characterization of monolith catalysts loaded with copper and manganese for low-temperature NH₃-SCR[J]. J Fuel Chem Technol, 2009, 37(5): 588-594.

TIAN L, YE D, LIANG H. Catalytic performance of novel ceramic-supported vanadium oxide catalyst for NO reduction with NH₃[J]. Catal Today, 2003, 78(1/4): 159-170.

CHOI S H, CHO S P, LEE J Y, HONG S H, HONG S-I. The inuence of non-stoichiometric species of V/TiO₂ catalysts on selective catalytic reduction at low temperature[J]. J Mol Catal A, 2009, 304(1/2): 166-173.

NICOSIA D, CZEKAJ I, KRCHER O. Chemical deactivation of V₂O₅/WO₃-TiO₂ SCR catalysts by additives and impurities from fuels, lubrication oils and urea solution: Part II Characterization study of the effect of alkali and alkaline earth metals[J]. Appl Catal B, 2008, 77(3/4): 228-236.

KOBAYASHI M, KUMA R, MASAKI S, SUGISHIMA N. TiO₂-SiO₂ and V₂O₅/TiO₂-SiO₂ catalyst: Physico-chemical characteristics and catalytic behavior in selective catalytic reduction of NO by NH₃[J]. Appl Catal B, 2005, 60(3/4): 173-179.

LZARO M J, BOYANO A, HERRERA C, LARRUBIA M A, ALEMANY L J, MOLINER R. Vanadium loaded carbon-based monoliths for the on-board NO reduction: Inuence of vanadia and tungsten loadings[J]. Chem Eng J, 2009, 155(1/2): 68-75.

BENNICI S, CARNITI P, GERVASINI A. Bulk and surface properties of dispersed CuO phases in relation with activity of NO_x reduction[J]. Catal Lett, 2004, 98(4): 187-194.

SREEKANTH P M, PEA D A, SMIRNIOTIS P G. Titania supported bimetallic transition metal oxides for low-temperature SCR of NO with NH₃[J]. Ind Eng Chem Res, 2006, 45(19): 6444-6449.

PUTLURU S S R, RIISAGER A, FEHRMANN R. The effect of acidic and redox properties of V₂O₅/CeO₂-ZrO₂ catalysts in selective catalytic reduction of NO by NH₃[J]. Catal Lett, 2009, 133(3/4): 370-375.

REICHE M A, MACIEJEWSKI M, BAIKER A. Characterization by temperature programmed reduction[J]. Catal Today, 2000, 56(4): 347-355.

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