In situ FT-IR study of Rh-Al-MCM-41 catalyst for the selective catalytic reduction of nitric oxide with propylene in the presence of excess oxygen

被引:41
作者
Long, RQ [1 ]
Yang, RT [1 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
来源
JOURNAL OF PHYSICAL CHEMISTRY B | 1999年 / 103卷 / 12期
关键词
D O I
10.1021/jp984525d
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
Rh-exchanged Al-MCM-41 is studied for selective catalytic reduction (SCR) of NO by C3H6 in the presence of excess oxygen. It shows a high activity in converting NO to N-2 and N2O at low temperatures. In situ FT-IR studies indicate that Rh-NO+ species (1910-1898 cm(-1)) is formed on the Rh-A1-MCM-41 catalyst in flowing NO/He, NO + O-2/He and NO + C3H6 + O-2/He at 100-350 degrees C. This species is quite active in reacting with propylene and/or propylene adspecies (e.g., pi-C3H5, polyene, etc.) at 250 degrees C in the presence/absence of oxygen, leading to the formation of the isocyanate species (Rh-NCO, at 2174 cm(-1)), CO, and CO2. Rh-NCO is also detected under reaction conditions. A possible reaction pathway for reduction of NO by C3H6 is proposed. In the SCR reaction, Rh-NO+ and propylene adspecies react to generate the Rh-NCO species, then Rh-NCO reacts with O-2, NO, and NO2 to produce N-2, N2O, and CO2. Rh-NO+ and Rh-NCO species are two main intermediates for the SCR reaction on Rh-Al-MCM-41 catalyst.
引用
收藏
页码:2232 / 2238
页数:7
相关论文
共 32 条
  • [1] Selective catalytic reduction of nitric oxide by hydrocarbons
    Amiridis, MD
    Zhang, TJ
    Farrauto, RJ
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 10 (1-3) : 203 - 227
  • [2] INFRARED STUDY OF NITRIC-OXIDE ADSORBED ON RHODIUM-ALUMINA CATALYST
    ARAI, H
    TOMINAGA, H
    [J]. JOURNAL OF CATALYSIS, 1976, 43 (1-3) : 131 - 142
  • [3] NO adsorption, desorption, and reduction by CH4 over Mn-ZSM-5
    Aylor, AW
    Lobree, LJ
    Reimer, JA
    Bell, AT
    [J]. JOURNAL OF CATALYSIS, 1997, 170 (02) : 390 - 401
  • [4] AN FTIR STUDY OF THE SPECIES ADSORBED ON A RH/AL2O3 CATALYST IN THE SELECTIVE REDUCTION OF NO BY PROPYLENE
    BAMWENDA, GR
    OBUCHI, A
    OGATA, A
    MIZUNO, K
    [J]. CHEMISTRY LETTERS, 1994, (11) : 2109 - 2112
  • [5] SELECTIVE REDUCTION OF NITRIC-OXIDE WITH PROPENE OVER PLATINUM-GROUP BASED CATALYSTS - STUDIES OF SURFACE SPECIES AND CATALYTIC ACTIVITY
    BAMWENDA, GR
    OGATA, A
    OBUCHI, A
    OI, J
    MIZUNO, K
    SKRZYPEK, J
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1995, 6 (04) : 311 - 323
  • [6] Synthesis and characterization of mesostructured materials
    Biz, S
    Occelli, ML
    [J]. CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1998, 40 (03): : 329 - 407
  • [7] SYNTHESIS OF ALUMINUM-RICH MCM-41
    BORADE, RB
    CLEARFIELD, A
    [J]. CATALYSIS LETTERS, 1995, 31 (2-3) : 267 - 272
  • [8] Mechanistic considerations for the reduction of NOx over Pt/Al2O3 and Al2O3 catalysts under lean-burn conditions
    Burch, R
    Sullivan, JA
    Watling, TC
    [J]. CATALYSIS TODAY, 1998, 42 (1-2) : 13 - 23
  • [9] MECHANISM OF THE SELECTIVE REDUCTION OF NITROGEN MONOXIDE ON PLATINUM-BASED CATALYSTS IN THE PRESENCE OF EXCESS OXYGEN
    BURCH, R
    MILLINGTON, PJ
    WALKER, AP
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 4 (01) : 65 - 94
  • [10] PROPYLENE AND OXYGEN CHEMISORPTION ON CUPRIC OXIDE AND CUPROUS OXIDE CATALYSTS
    GEREI, SV
    ROZHKOVA, EV
    GOROKHOV.YB
    [J]. JOURNAL OF CATALYSIS, 1973, 28 (03) : 341 - 350