Preparation and performance of V-W/<em>x</em>(Mn-Ce-Ti)/<em>y</em>(Cu-Ce-Ti)/cordierite catalyst by impregnation method in sequence for SCR reaction with urea

DONG Guo-jun; ZHAO Yuan; ZHANG Yu-feng

Volume 42 Issue 09

Sep. 2014

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2014 > 42(09): 1093-1101

DONG Guo-jun, ZHAO Yuan, ZHANG Yu-feng. Preparation and performance of V-W/x(Mn-Ce-Ti)/y(Cu-Ce-Ti)/cordierite catalyst by impregnation method in sequence for SCR reaction with urea[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1093-1101.

Citation:

DONG Guo-jun, ZHAO Yuan, ZHANG Yu-feng. Preparation and performance of V-W/x(Mn-Ce-Ti)/y(Cu-Ce-Ti)/cordierite catalyst by impregnation method in sequence for SCR reaction with urea[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1093-1101.

Citation:

DONG Guo-jun, ZHAO Yuan, ZHANG Yu-feng. Preparation and performance of V-W/x(Mn-Ce-Ti)/y(Cu-Ce-Ti)/cordierite catalyst by impregnation method in sequence for SCR reaction with urea[J]. Journal of Fuel Chemistry and Technology, 2014, 42(09): 1093-1101.

PDF( 924 KB)

Preparation and performance of V-W/x(Mn-Ce-Ti)/y(Cu-Ce-Ti)/cordierite catalyst by impregnation method in sequence for SCR reaction with urea

College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China

Funds: Supported by Fundamental Research Funds for the Central Universities (HEUCF20136910012) and Advanced Technique Project Funds of the Manufacture and Information Ministry.

Received Date: 2014-04-11
Rev Recd Date: 2014-06-14
Publish Date: 2014-09-30

Abstract

Abstract

Mn-Ce/TiO₂ (M) and Cu-Ce/TiO₂ (C) were prepared by sol-gel method, and the cordierite honeycomb ceramics (CC) was coated with M and/or C and V₂O₅-WO₃ in sequence by impregnation method. A series of monolith catalysts were evaluated for the selective catalytic reduction (SCR) of NO_x by urea. The physical and chemical properties of the catalysts were well examined using nitrogen adsorption, CO₂-TPD, NH₃-TPD, XRD, XPS and H₂-TPR experiments. The results showed that when the M phase was coated onto catalyst prior to C phase, the complex catalyst V/3C/3M/CC was more active than the catalysts with only M or C phase in the presence of 0.01% SO₂ and 10% H₂O, and a small quantity of SO₂ may favor the urea-SCR activity. XRD analysis indicated that Cu, Ce modified TiO₂ sol favors the formation of anatase phase, and Mn, Ce modified TiO₂ sol facilitates the formation of rutile phase. The BET surface area of catalyst only has relationship with the amount of M or C phase, and loading sequence does not influence it so much. The introduction of M phase and C phase increases the surface acid sites of different intensity. H₂-TPR results showed the interaction between vanadium and copper and/or manganese species enhances the reduction of vanadium, which can increase the amount of H₂ consumption. XPS results indicated that both high V⁴⁺/V⁵⁺ ratio and large amount of surface chemisorbed oxygen may beneficial to the activity of the catalysts.
- urea-SCR,
- NO_x,
- V₂O₅-WO₃/TiO₂,
- Mn,
- Cu

FullText(HTML)

References(45)

References

BOSCH H, JANSSEN F. Formation and control of nitrogen oxides[J]. Catal Today, 1988, 2(4): 369-379.

BUSCA G, LIETTI 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.

FORZATTI P. Present status and perspectives in de-NO_x SCR catalysis[J]. Appl Catal A: Gen, 2001, 222(1/2): 221-236.

BUSCA G, LARRUBIA M A, ARRIGHI L, RAMIS G. Catalytic abatement of NO_x : Chemical and mechanistic aspects[J]. Catal Today, 2005, 107-108(30): 139-148.

KOEBEL M, ELSENER M, KLEEMANN M. Urea-SCR: A promising technique to reduce NO_x emissions from automotive diesel engines[J]. Catal Today, 2000, 59(3/4): 335-345.

LIETTI L, FORZATTI P, BREGANI F. Steady-state and transient reactivity study of TiOâ-supported VâOâ-WOâ De-NOâ catalysts: Relevance of the vanadium-tungsten interaction on the catalytic activity[J]. Ind Eng Chem Res, 1996, 35(11): 3884-3892.

CHEN J P, YANG R T. Role of WO₃ in mixed V₂O₅-WO₃/TiO₂ catalysts for selective catalytic reduction of nitric oxide with ammonia[J]. Appl Catal A: Gen, 1992, 80(1/2): 135-148.

THIRUPATHI B, SMIRNIOTIS P G. Nickel-doped Mn/TiO₂ as an efficient catalyst for the low-temperature SCR of NO with NH₃: Catalytic evaluation and characterizations[J]. J Catal, 2012, 288(1): 74-83.

POURKHALIL M, MOGHADDAM A Z, RASHIDI A, TOWFIGHI J, MORTAZAVI Y. Preparation of highly active manganese oxides supported on functionalized MWNTs for low temperature NO_x reduction with NH₃[J]. Appl Surf Sci, 2013, 279: 250-259.

WANG C Z, YANG S J, CHANG H Z, PENG Y, LI J H. Structural effects of iron spinel oxides doped with Mn, Co, Ni and Zn on selective catalytic reduction of NO with NH₃[J]. J Mol Catal A: Chem, 2013, 376: 13-21.

LEE S M, PARK K H, HONG S C. MnO_x/CeO₂-TiO₂ mixed oxide catalysts for the selective catalytic reduction of NO with NH₃ at low temperature[J]. Chem Eng J, 2012, 195-196: 323-331.

WANG X, ZHENG Y Y, LIN J X. Highly dispersed Mn-Ce mixed oxides supported on carbon nanotubes for low-temperature NO reduction with NH₃[J]. Catal Commun, 2013, 37: 96-99.

LI J F, YAN N Q, QU Z, QIAO S H, YANG S J, GUO Y F, LIU P, JIA J P. Catalytic oxidation of elemental mercury over the modified catalyst Mn/α-Al₂O₃ at lower temperatures[J]. Environ Sci Technol, 2010, 44(1): 426-431.

PEÑA D A, UPHADE B, 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.

TANG N, LIU Y, WANG H, WU Z. Mechanism study of NO catalytic oxidation over MnO_x/TiO₂ Catalysts[J]. J Phys Chem C, 2011, 115(16): 8214-8220.

DU X S, GAO X, CUI L W, FU Y C, LUO Z Y, CEN K F. Investigation of the effect of Cu addition on the SO₂-resistance of a Ce-Ti oxide catalyst for selective catalytic reduction of NO with NH₃[J]. Fuel, 2012, 92(1): 49-55.

WU Z B, JIN R B, WANG H Q, 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: 935-939.

JING Y, GAO X, WU W H. Effects of H₂O and SO₂ on the performance of V₂O₅/TiO₂ catalysts for selective catalytic reduction of NO in flue gas[J]. Proc CSEE, 2013, 30: 28-33.

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

KRÖCHER O, ELSENER M. Combination of V₂O₅/WO₃-TiO₂, Fe-ZSM5, and Cu-ZSM5 catalysts for the selective catalytic reduction of nitric oxide with ammonia[J]. Ind Eng Chem Res, 2008, 47(22): 8588-8593.

黄妍, 童志权, 伍斌, 张俊丰. V₂O₅-CeO₂/TiO₂催化剂上低温氨选择性催化还原NO的性能[J]. 燃料化学学报, 2008, 36(5): 616-620. (HUANG Yan, TONG Zhi-quan, WU Bing, ZHANG Jun-feng. Low temperature selective catalytic reduction of NO by ammonia over V₂O₅-CeO₂/TiO₂[J]. Journal of Fuel Chemistry and Technology, 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.

周超强, 董国君, 龚凡, 常雪. 铜锰复合低温NH₃-SCR整体催化剂的制备及其性能研究[J]. 燃料化学学报, 2009, 37(5): 588-594. (ZHOU Chao-qiang, DONG Guo-jun, GONG Fan, CHANG Xue. Preparation and characterization of monolith catalysts loaded with copper and manganese for low-temperature NH₃-SCR[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 588-594.)

WANG T J, BAEK S W, KWON H J, KIM Y J, NAM I S, CHA M S, YEO G K. Kinetic parameter estimation of a commercial Fe-zeolite SCR[J]. Ind Eng Chem Res, 2011, 50(5): 2850-2864.

FORZATTI P, NOVA I, TRONCONI E. Enhanced NH₃ selective catalytic reduction for NO_x abatement[J]. Angew Chem Int Edit, 2009, 121(44): 8516-8518.

ZHANG C P, ZHANG X L, WU X P, ZHANG L F, ZHANG H J, YANG B J. The mechanism of SO₂ influence on the denitration of MnO₂/PG catalysts at low temperature[J]. Acta Scientiae Circumstantiae, 2013, 33: 2686-2693.

WAQUIF M, BACHELIER J, SAUR O, LAVALLEY J C. Acidic properities and stability of sulfate-promoted metal oxides[J]. J Mol Catal, 1992, 72(1): 127-138.

CHEN J P, YANG R T. Selective catalytic reduction of NO with NH₃ on SO₄^2-/TiO₂ superacid catalyst[J]. J Catal, 1993, 139(1): 277-288.

SEO Y H, PRASETYANTO E A, JIANG N, OH S M, PARK S E. Catalytic dehydration of methanol over synthetic zeolite W[J]. Microporous Mesoporous Mater, 2010, 128(1/3): 108-114.

CHMIELARZ L, KUSTROWSKI P, ZBROJA M, KNAP B G, DATKA J, DZIEMBAJ R. SCR of NO by NH₃ on alumina or titania pillared montmorillonite modified with Cu or Co: Part Ⅱ. Temperature programmed studies[J]. Appl Catal B: Environ, 2004, 53(1): 47-61.

CHMIELARA L, KUSTROWSKI P, ZBROJA M, ?ASOCHA W, DZIEMBAJ R. Selective reduction of NO with NH3?over pillared clays modified with transition metals[J]. Catal Today, 2004, 90(1/2): 43-49.

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. Effect of Al₂O₃ promoter on a performance of C1-C14 α -alcohols direct synthesis over Co/AC catalysts via Fischer-Tropsch synthesis[J]. Catal Today, 2000, 56(4): 347-355.

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.

JEMAL J, TOUNSI H, DJEMEL S, PETTITO C, DELAHAY G. Characterization and deNO_x activity of copper-hydroxyapatite catalysts prepared by wet impregnation[J]. Reac Kinet Mech Cat, 2013, 109(1): 159-165.

WANG L, GAUDET J R, WEI L, WENG D. Migration of Cu species in Cu/SAPO-34 during hydrothermal aging[J]. J Catal, 2013, 306: 68-77.

CHOI S H, CHO S P, LEE JY, HONG S H, HONG S C, HONG S I. The influence 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.

LARACHI R, PIERRE J, ADNOT A, BERNIS A. Ce 3d XPS study of composite Ce_x Mn_1-xO_2-ywet oxidation catalysts[J]. Appl Surf Sci, 2002, 195(1/4): 236-250.

CARJA G, KAMESHIMA Y, OKADA K, MADHUSOODANA C D. Mn-Ce/ZSM5 as a new superior catalyst for NO reduction with NH₃[J]. Appl Catal B: Environ, 2007, 73(1/2): 60-64.

KANG M, PARK E D , KIM J M , YIE J E. Manganese oxide catalysts for NO_x reduction with NH₃ at low temperatures[J]. Appl Catal A: Gen, 2007, 327(2): 261-269.

PARK J H, PARK H J, BAIK J H, NAM I S, SHIN C H, LEE J H, CHO B K, OH S H. Hydrothermal stability of CuZSM5 catalyst in reducing NO by NH₃ for the urea selective catalytic reduction process[J]. J Catal, 2006, 240(1): 47-57.

KWAK J H, TOMKYN R G, KIM D H, SZANYI J, PEDEN C H F. Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NO_x with NH₃[J]. J Catal, 2010, 275(2): 187-190.

FICKEL D W, ADDIO E D, LAUTERBACH J A, LOBO R F. The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites[J]. Appl Catal B: Environ, 2011, 102(3/4): 441-448.

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: Environ, 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: Influence of vanadia and tungsten loadings[J]. Chem Eng J, 2009, 155(1/2): 68-75.

Relative Articles

Supplements(0)

Cited By

Proportional views