Selective catalytic reaction of NOx with NH3 over Ce-Fe/TiO2-loaded wire-mesh honeycomb: Resistance to SO2 poisoning

被引:124
作者
Shu, Yun [1 ]
Aikebaier, Tanana [1 ]
Quan, Xie [1 ]
Chen, Shuo [1 ]
Yu, Hongtao [1 ]
机构
[1] Dalian Univ Technol, Sch Environm Sci & Technol, Minist Educ, Key Lab Ind Ecol & Environm Engn, Dalian 116024, Peoples R China
关键词
SCR; Wire-mesh honeycomb catalyst; Surface sulfation; Resistance to SO2; LOW-TEMPERATURE SCR; CE/TIO2; CATALYST; REDUCTION; AMMONIA; MECHANISM; OXIDES; MN; FE; IRON; CE;
D O I
10.1016/j.apcatb.2014.01.008
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ce-Fe/TiO2/Al2O3/wire-mesh honeycomb catalyst (Ce-Fe/WMH) exhibited a high activity for the selective catalytic reduction (SCR) of NOx in SO2-containing gases. Analysis of fresh and spent catalysts by XRD, BET, XPS, TG and FTIR indicated that Ce sites were sulfated preferentially over Ce-Fe/WMH during the SCR reaction in the presence of SO2, which could increase the amount of surface active oxygen species. On the other hand, the formation of surface hydroxyls due to the hydration of SO42- could supply more Bronsted acid sites to adsorb NH3 in the form of NH4+. These two factors played significant roles in the good SO2 durability of Ce-Fe/WMH. In addition, the sulfation of CeO2 on catalyst surface might approach a stable state upon certain amount of SO2 in reactant gas. The reaction mechanism study showed that only Eley-Rideal reaction pathway between ionic NH4+, coordinated NH3 and gaseous NO dominated in the reaction; the Langmuir-Hinshelwood reaction pathway was cut off by the sulfation, resulting in the rapid decrease of NOx conversion in the early period of SCR reaction in the presence of SO2. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:630 / 635
页数:6
相关论文
共 44 条
  • [1] Characterization and composition of commercial V2O5-WO3-TiO2 SCR catalysts
    Alemany, LJ
    Berti, F
    Busca, G
    Ramis, G
    Robba, D
    Toledo, GP
    Trombetta, M
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 10 (04) : 299 - 311
  • [2] Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:: A review
    Busca, G
    Lietti, L
    Ramis, G
    Berti, F
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 18 (1-2) : 1 - 36
  • [3] SELECTIVE CATALYTIC REDUCTION OF NO WITH NH3 ON SO4(-2)/TIO2 SUPERACID CATALYST
    CHEN, JP
    YANG, RT
    [J]. JOURNAL OF CATALYSIS, 1993, 139 (01) : 277 - 288
  • [4] The different impacts of SO2 and SO3 on Cu/zeolite SCR catalysts
    Cheng, Yisun
    Lambert, Christine
    Kim, Do Heui
    Kwak, Ja Hun
    Cho, Sung June
    Peden, Charles H. F.
    [J]. CATALYSIS TODAY, 2010, 151 (3-4) : 266 - 270
  • [5] Systematic XPS studies of metal oxides, hydroxides and peroxides
    Dupin, JC
    Gonbeau, D
    Vinatier, P
    Levasseur, A
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (06) : 1319 - 1324
  • [6] Concentration of Ce3+ and oxygen vacancies in cerium oxide nanoparticles
    Dutta, P.
    Pal, S.
    Seehra, M. S.
    Shi, Y.
    Eyring, E. M.
    Ernst, R. D.
    [J]. CHEMISTRY OF MATERIALS, 2006, 18 (21) : 5144 - 5146
  • [7] Role of sulphates on the mechanism of NH3-SCR of NO at low temperatures over presulphated vanadium supported on carbon-coated monoliths
    García-Bordejé, E
    Pinilla, JL
    Lázaro, MJ
    Moliner, R
    Fierro, JLG
    [J]. JOURNAL OF CATALYSIS, 2005, 233 (01) : 166 - 175
  • [8] Air-liquid interfaces of aqueous solutions containing ammonium and sulfate: Spectroscopic and molecular dynamics studies
    Gopalakrishnan, S
    Jungwirth, P
    Tobias, DJ
    Allen, HC
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (18) : 8861 - 8872
  • [9] Selective Catalytic Reduction of NOx with NH3 over Mn, Ce Substitution Ti0.9V0.1O2-δ Nanocomposites Catalysts Prepared by Self-Propagating High-Temperature Synthesis Method
    Guan, Bin
    Lin, He
    Zhu, Lin
    Huang, Zhen
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (26) : 12850 - 12863
  • [10] Defective structure, oxygen mobility, oxygen storage capacity, and redox properties of RE-based (RE = Ce, Pr) solid solutions
    He, H
    Dai, H
    Au, CT
    [J]. CATALYSIS TODAY, 2004, 90 (3-4) : 245 - 254