Location and activity of VOx species on TiO2 particles for NH3-SCR catalysis

被引:65
作者
Ganjkhanlou, Yadolah [1 ]
Janssens, Ton V. W. [2 ]
Vennestrom, Peter N. R. [2 ]
Mino, Lorenzo [1 ]
Paganini, Maria Cristina [1 ]
Signorile, Matteo [1 ]
Bordiga, Silvia [1 ]
Berlier, Gloria [1 ]
机构
[1] Univ Torino, NIS & INSTM Ctr, Dept Chem, Via P Giuria 7, I-10125 Turin, Italy
[2] Umicore Denmark ApS, Nojsomhedsvej 20, DK-2800 Lyngby, Denmark
关键词
VOx-TiO2; catalyst; NH3-SCR; Infrared spectroscopy; Electron paramagnetic resonance; CO adsorption; VANADIA-TITANIA CATALYSTS; IN-SITU RAMAN; TEMPERATURE CO ADSORPTION; OXIDE CATALYSTS; NITRIC-OXIDE; MOLECULAR-STRUCTURES; SURFACE-PROPERTIES; SUPPORTED VANADIA; IR SPECTROSCOPY; FT-IR;
D O I
10.1016/j.apcatb.2020.119337
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
The role of anatase TiO2 on the performance of VOx-TiO2 is studied by in situ spectroscopies on a series of catalysts with 1.9-9.7 V at/nm(2). At low coverages, VOx is preferentially located at defect sites, spreading on the main TiO2 {101} and {100} facets at intermediate coverages. Bronsted sites concentration is maximum around 6 V atoms/nm(2), and EPR shows a significant amount of V4+ at intermediate VOx densities, indicating the influence of TiO2 on their reducibility. The activity is proportional to the square of the VOx density up to 5.8 V atoms/nm(2). All catalysts show the same activation energy for NH3-SCR of 56.9 +/- 1.0 kJ/mol in the temperature range 160-280 degrees C, indicating that the reaction path does not change in the studied V coverage range. The activity does not follow the observed trends for Bronsted acid sites or reducibility, and it seems that the ability to form V-pairs is the only requirement for catalytic activity.
引用
收藏
页数:10
相关论文
共 92 条
  • [1] The reaction mechanism for the SCR process on monomer V5+ sites and the effect of modified Bronsted acidity
    Arnarson, Logi
    Falsig, Hanne
    Rasmussen, Soren B.
    Lauritsen, Jeppe V.
    Moses, Poul Georg
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (25) : 17071 - 17080
  • [2] Coexistence of Square Pyramidal Structures of Oxo Vanadium (+5) and (+4) Species Over Low-Coverage VOX/TiO2 (101) and (001) Anatase Catalysts
    Arnarson, Logi
    Rasmussen, Soren B.
    Falsig, Hanne
    Lauritsen, Jeppe V.
    Moses, Poul Georg
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (41) : 23445 - 23452
  • [3] Synthesis and characterization of alumina-supported vanadium oxide catalysts prepared by the molecular designed dispersion of VO(acac)2 complexes
    Baltes, M
    Van Der Voort, P
    Weckhuysen, BM
    Rao, RR
    Catana, G
    Schoonheydt, RA
    Vansant, EF
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (11) : 2673 - 2680
  • [4] Molecular structures of supported metal oxide catalysts under different environments
    Bañares, MA
    Wachs, IE
    [J]. JOURNAL OF RAMAN SPECTROSCOPY, 2002, 33 (05) : 359 - 380
  • [5] Dynamic behavior of supported vanadia catalysts in the selective oxidation of ethane -: In situ Raman, UV-Vis DRS and reactivity studies
    Bañares, MA
    Martínez-Huerta, MV
    Gao, X
    Fierro, JLG
    Wachs, IE
    [J]. CATALYSIS TODAY, 2000, 61 (1-4) : 295 - 301
  • [6] Surfactant templated synthesis of porous VOx-ZrO2 catalysts for ethanol conversion to acetaldehyde
    Boldog, Ishtvan
    Cicmanec, Pavel
    Ganjkhanlou, Yadolah
    Bulanek, Roman
    [J]. CATALYSIS TODAY, 2018, 304 : 64 - 71
  • [7] Assessing the acidity of high silica chabazite H-SSZ-13 by FTIR using CO as molecular probe: Comparison with H-SAPO-34
    Bordiga, S
    Regli, L
    Cocina, D
    Lamberti, C
    Bjorgen, M
    Lillerud, KP
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (07) : 2779 - 2784
  • [8] CO and NO adsorption on VOx/SBA-15 catalysts: an FT-IR spectroscopic study
    Bulanek, R.
    Drenchev, N.
    Cicmanec, P.
    Setnicka, M.
    [J]. ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY, 2013, 19 (2-4): : 339 - 347
  • [9] CHEMICAL AND SPECTROSCOPIC STUDY OF THE NATURE OF A VANADIUM-OXIDE MONOLAYER SUPPORTED ON A HIGH-SURFACE-AREA TIO2 ANATASE
    BUSCA, G
    CENTI, G
    MARCHETTI, L
    TRIFIRO, F
    [J]. LANGMUIR, 1986, 2 (05) : 568 - 577
  • [10] FT-IR STUDY OF THE SURFACE-PROPERTIES OF POLYCRYSTALLINE VANADIA
    BUSCA, G
    RAMIS, G
    LORENZELLI, V
    [J]. JOURNAL OF MOLECULAR CATALYSIS, 1989, 50 (02): : 231 - 240