全部 标题 作者
关键词 摘要

OALib Journal期刊
ISSN: 2333-9721
费用:99美元

查看量下载量

相关文章

更多...
科学通报  2014 

不同Ce/Zr摩尔比对Fe2O3-WO3/CexZr1-xO2(0≤x≤1)整体式催化剂的NH3选择性催化还原NOx性能的影响

DOI: 10.1360/csb2014-59-26-2550, PP. 2550-2559

Keywords: 选择性催化还原,氮氧化物,摩尔比,Fe2O3-WO3,CexZr1-xO2

Full-Text   Cite this paper   Add to My Lib

Abstract:

以共沉淀法合成了一系列不同Ce/Zr摩尔比的CexZr1-xO2(0≤x≤1)复合氧化物载体,并制备了一系列Fe2O3-WO3/CexZr1-xO2整体式催化剂用于NH3选择性催化还原NOx(NH3-SCR).通过N2物理吸附,X射线衍射(XRD),X射线光电子能谱(XPS)和H2程序升温还原(H2-TPR)表征了催化剂的结构性质和氧化还原性能,并测试了各催化剂的NH3-SCR活性.结果表明,催化剂的NH3-SCR性能随着Ce/Zr摩尔比的增大而逐渐提高,尤其是低温催化活性和反应温度窗口.在所考察的催化剂中,Fe2O3-WO3/Ce0.68Zr0.32O2表现出最高的NH3-SCR活性,在247~454℃温度范围内,该催化剂在30000h-1空速下可将90%以上的NOx有效净化;且在整个反应窗口内该催化剂的N2选择性均超过99%,而生成的N2O浓度则小于20ppm(1ppm=10-6L/L),并且表现出较强的抗水抗硫性能、优异的织构和结构性能.更多的表面Fe,Ce和活性氧物种的共同作用,使得Fe2O3-WO3/Ce0.68Zr0.32O2具有优异的NH3-SCR性能.

References

[1]  2 Balle P, Geiger B, Kureti S. Selective catalytic reduction of NOx by NH3 on Fe/HBEA zeolite catalysts in oxygen-rich exhaust. Appl Catal B, 2009, 85: 109-119
[2]  3 张秋林, 邱春天, 徐海迪, 等. 整体式 Cu-ZSM-5 催化剂上 NH3 选择性催化还原 NO 活性. 催化学报, 2010, 31: 1411-1416
[3]  4 Kwak J H, Tonkyn R G, Kim D H, et al. Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3. J Catal, 2010, 275: 187-190
[4]  7 Collier J E, Laroze S C, Rajaram R R, et al. Non-zeolite base metal SCR catalyst. USA Patent, US7985391 B2, 2011-06-26
[5]  10 Pietrogiacomi D, Magliano A, Sannino D, et al. In situ sulphated CuOx/ZrO2 and CuOx/sulphated-ZrO2 as catalysts for the reduction of NOx with NH3 in the presence of excess O2. Appl Catal B, 2005, 60: 83-92
[6]  11 Xu H, Zhang Q, Qiu C, et al. Tungsten modified MnOx-CeO2/ZrO2 monolith catalysts for selective catalytic reduction of NOx with ammonia. Chem Eng Sci, 2012, 76: 120-128
[7]  13 Li Y, Cheng H, Li D, et al. WO3/CeO2-ZrO2, a promising catalyst for selective catalytic reduction (SCR) of NOx with NH3 in diesel exhaust. Chem Commun, 2008, 1470-1472
[8]  22 Apostolescu N, Geiger B, Hizbullah K, et al. Selective catalytic reduction of nitrogen oxides by ammonia on iron oxide catalysts. Appl Catal B, 2006, 62: 104-114
[9]  23 Chen L, Li J, Ge M, et al. Enhanced activity of tungsten modified CeO2/TiO2 for selective catalytic reduction of NOx with ammonia. Catal Today, 2010, 153: 77-83
[10]  24 Khodayari R, Odenbrand C U I. Regeneration of commercial TiO2-V2O5-WO3 SCR catalysts used in bio fuel plants. Appl Catal B, 2001, 30: 87-99
[11]  32 Martínez A, Prieto G, Arribas M A, et al. Influence of the preparative route on the properties of WOx-ZrO2 catalysts: A detailed structural, spectroscopic, and catalytic study. J Catal, 2007, 248: 288-302
[12]  33 Liu F, He H, Ding Y, et al. Effect of manganese substitution on the structure and activity of iron titanate catalyst for the selective catalytic reduction of NO with NH3. Appl Catal B, 2009, 93: 194-204
[13]  39 Wu Z, Jin R, Wang H. Ceria modified MnOx/TiO2 as a superior catalyst for NO reduction with NH3 at low-temperature. Catal Commun, 2008, 9: 2217-2220
[14]  40 Kang M, Park E D, Kim J M, et al. Manganese oxide catalysts for NOx reduction with NH3 at low temperatures. Appl Catal A, 2007, 327: 261-269
[15]  41 Si Z, Weng D, Wu X, et al. NH3-SCR activity, hydrothermal stability, sulfur resistance and regeneration of Ce0.75Zr0.25O2-PO43-catalyst. Catal Commun, 2012, 17: 146-149
[16]  42 Ma Z, Weng D, Wu X, et al. Effects of WOx modification on the activity, adsorption and redox properties of CeO2 catalyst for NOx reduction with ammonia. J Environ Sci, 2012, 24: 1305-1316
[17]  43 Barton D G, Soled S L, Meitzner G D, et al. Structural and catalytic characterization of solid acids based on zirconia modified by tungsten oxide. J Catal, 1999, 181: 57-72
[18]  44 Liu F, He H. Structure-activity relationship of iron titanate catalysts in the selective catalytic reduction of NOx with NH3. J Phys Chem C, 2010, 114: 16929-16936
[19]  1 Busca G, Larrubia M A, Arrighi L, et al. Catalytic abatement of NOx: Chemical and mechanistic aspects. Catal Today, 2005, 107-108: 139-148
[20]  5 Picone A L, Warrender S J, Slawin A M Z, et al. A co-templating route to the synthesis of Cu SAPO STA-7, giving an active catalyst for the selective catalytic reduction of NO. Micropor Mesopor Mat, 2011, 146: 36-47
[21]  6 Deka U, Lezcano-Gonzalez I, Warrender S J, et al. Changing active sites in Cu-CHA catalysts: deNOx selectivity as a function of the preparation method. Micropor Mesopor Mat, 2013, 166: 144-152
[22]  8 Qi G, Yang R T. A superior catalyst for low-temperature NO reduction with NH3. Chem Commun, 2003, 848-849
[23]  9 Gao X, Jiang Y, Fu Y, et al. Preparation and characterization of CeO2/TiO2 catalysts for selective catalytic reduction of NO with NH3. Catal Commun, 2010, 11: 465-469
[24]  12 Murota T, Hasegawa T, Aozasa S, et al. Production method of cerium oxide with high storage capacity of oxygen and its mechanism. J Alloys Compd, 1993, 193: 298-299
[25]  14 Si Z, Weng D, Wu X, et al. Modifications of CeO2-ZrO2 solid solutions by nickel and sulfate as catalysts for NO reduction with ammonia in excess O2. Catal Commun, 2010, 11: 1045-1048
[26]  15 Xu H, Wang Y, Cao Y, et al. Catalytic performance of acidic zirconium-based composite oxides monolithic catalyst on selective catalytic reduction of NOx with NH3. Chem Eng J, 2014, 240: 62-73
[27]  16 Shen B, Wang Y, Wang F, et al. The effect of Ce-Zr on NH3-SCR activity over MnOx(0.6)/Ce0.5Zr0.5O2 at low temperature. Chem Eng J, 2014, 236: 171-180
[28]  17 Ramis G, Yi L, Busca G, et al. Adsorption, activation, and oxidation of ammonia over SCR catalysts. J Catal, 1995, 157: 523-535
[29]  18 Cheng L S, Yang R T, Chen N. Iron oxide and chromia supported on titania-pillared clay for selective catalytic reduction of nitric oxide with ammonia. J Catal, 1996, 164: 70-81
[30]  19 Long R Q, Yang R T. Catalytic performance of Fe-ZSM-5 catalysts for selective catalytic reduction of nitric oxide by ammonia. J Catal, 1999, 188: 332-339
[31]  20 Chen J P, Yang R T. Role of WO3 in mixed V2O5-WO3/TiO2 catalysts for selective catalytic reduction of nitric oxide with ammonia. Appl Catal A, 1992, 80: 135-148
[32]  21 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. Appl Catal B, 1998, 18: 1-36
[33]  25 Wang J, Wen J, Shen M. Effect of interaction between Ce0.7Zr0.3O2 and Al2O3 on structural characteristics, thermal stability, and oxygen storage capacity. J Phys Chem C, 2008, 112: 5113-5122
[34]  26 Theocharis C, Kyriacou G, Christophidou M. Preparation and characterization of nanoporous ceria containing heteroatoms, with and without a matrix. Adsorption, 2005, 11: 763-767
[35]  27 Alifanti M, Baps B, Blangenois N, et al. Characterization of CeO2-ZrO2 mixed oxides. Comparison of the citrate and sol-gel preparation methods. Chem Mater, 2003, 15: 395-403
[36]  28 He H, Dai H X, Au C T. Defective structure, oxygen mobility, oxygen storage capacity, and redox properties of RE-based (RE = Ce, Pr) solid solutions. Catal Today, 2004, 90: 245-254
[37]  29 Noronha F B, Fendley E C, Soares R R, et al. Correlation between catalytic activity and support reducibility in the CO2 reforming of methane over Pt/CexZr1-xO2 catalysts. Chem Eng J, 2001, 82: 21-31
[38]  30 Gu T, Jin R, Liu Y, et al. Promoting effect of calcium doping on the performances of MnOx/TiO2 catalysts for NO reduction with NH3 at low temperature. Appl Catal B, 2013, 129: 30-38
[39]  31 Xu H, Fang Z, Cao Y, et al. Influence of Mn/(Mn+Ce) ratio of MnOx-CeO2/WO3-ZrO2 monolith catalyst on selective catalytic reduction of NOx with ammonia. Chin J Catal, 2012, 33: 1927-1937
[40]  34 Ardizzone S, Bianchi C L, Signoretto M. Zr(IV) surface chemical state and acid features of sulphated-zirconia samples. Appl Surf Sci, 1998, 136: 213-220
[41]  35 Ardizzone S, Bianchi C L. XPS characterization of sulphated zirconia catalysts: The role of iron. Surf Interface Anal, 2000, 30: 77-80
[42]  36 Gao S, Chen X, Wang H, et al. Ceria supported on sulfated zirconia as a superacid catalyst for selective catalytic reduction of NO with NH3. J Colloid Interface Sci, 2013, 394: 515-521
[43]  37 Fang J, Bi X, Si D, et al. Spectroscopic studies of interfacial structures of CeO2-TiO2 mixed oxides. Appl Surf Sci, 2007, 253: 8952-8961
[44]  38 Shan W, Liu F, He H, et al. A superior Ce-W-Ti mixed oxide catalyst for the selective catalytic reduction of NOx with NH3. Appl Catal B, 2012, 115-116: 100-106

Full-Text

Contact Us

service@oalib.com

QQ:3279437679

WhatsApp +8615387084133