Mechanistic features for propane reforming by carbon dioxide over a Ni/Mg(Al)O hydrotalcite-derived catalyst

被引:69
作者
Olafsen, A
Slagern, Å
Dahl, IM
Olsbye, U
Schuurman, Y
Mirodatos, C
机构
[1] Univ Oslo, Ctr Mat Sci & Nanotechnol, Dept Chem, N-0315 Oslo, Norway
[2] Inst Rech Catalyse, CNRS, F-69626 Villeurbanne, France
[3] SINTEF, Mat & Chem, N-0314 Oslo, Norway
关键词
CO2; reforming; propane; hydrotalcite; mechanistic study; magnetic measurements; DRIFTS TAP; TEM; metal-support interaction;
D O I
10.1016/j.jcat.2004.10.002
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
A 1.9 wt% Ni/Mg(Al)O hydrotalcite-derived catalyst is Studied for the dry reforming of propane to synthesis gas at 600 degreesC and 1 atm. The catalyst showed limited initial deactivation and then was exceptionally stable throughout a 34-day test. Catalyst characterisation indicates that the carrier material consists of a mixed Mg(Al)O phase before and after testing, and that carbonate forms on the support surface under dry reforming conditions. The Ni particles are in close contact with, and partially decorated by, the basic support. No carbon whisker formation is observed by transmission electron microscopy after catalytic testing. Alternating pulse experiments in a Temporary Analysis of Product-II (TAP-II) reactor system indicate that CO2 is associatively adsorbed on the basic Mg(Al)O carrier and acts as a permanent Source of oxygen species for the Ni metal. Propane reacts rapidly with Ni-O species to form CO and H2O. Under TAP conditions, reduced Ni reacts gradually with carbonate from the support to give Ni-O species and CO. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:163 / 175
页数:13
相关论文
共 27 条
  • [1] [Anonymous], 2020, CATAL SCI TECHNOL
  • [2] The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis
    Bligaard, T
    Norskov, JK
    Dahl, S
    Matthiesen, J
    Christensen, CH
    Sehested, J
    [J]. JOURNAL OF CATALYSIS, 2004, 224 (01) : 206 - 217
  • [3] HYDROTALCITE-TYPE ANIONIC CLAYS: PREPARATION, PROPERTIES AND APPLICATIONS
    Cavani, F.
    Trifiro, F.
    Vaccari, A.
    [J]. CATALYSIS TODAY, 1991, 11 (02) : 173 - 301
  • [4] DALMON JA, 1994, CATALYST CHARACTERIZ
  • [5] TAP study of the mechanism and kinetics of the adsorption and combustion of methane on Ni/Al2O3 and NiO/Al2O3
    Dewaele, O
    Froment, GF
    [J]. JOURNAL OF CATALYSIS, 1999, 184 (02) : 499 - 513
  • [6] Equilibria and kinetics of CO2 adsorption on hydrotalcite adsorbent
    Ding, Y
    Alpay, E
    [J]. CHEMICAL ENGINEERING SCIENCE, 2000, 55 (17) : 3461 - 3474
  • [7] Adsorption-enhanced steam-methane reforming
    Ding, Y
    Alpay, E
    [J]. CHEMICAL ENGINEERING SCIENCE, 2000, 55 (18) : 3929 - 3940
  • [8] CO2 coordination to nickel atoms: Matrix isolation and density functional studies
    Galan, F
    Fouassier, M
    Tranquille, M
    Mascetti, J
    Papai, I
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 1997, 101 (14) : 2626 - 2633
  • [9] TAP-2: An interrogative kinetics approach
    Gleaves, JT
    Yablonskii, GS
    Phanawadee, P
    Schuurman, Y
    [J]. APPLIED CATALYSIS A-GENERAL, 1997, 160 (01) : 55 - 88
  • [10] *INT UN PUR APPL C, 1961, MOL STRUCT SPECTR