Catalytic production of methane from CO2 and H2 at low temperature Insight on the reaction mechanism

被引:171
作者
Jacquemin, Marc [1 ]
Beuls, Antoine [1 ]
Ruiz, Patricio [1 ]
机构
[1] Catholic Univ Louvain, Inst Condensed Matter & Nanosci, IMCN, Div Mol Solids & React MOST, B-1348 Louvain, Belgium
关键词
CO2; Methanation; Dissociation; DRIFT spectroscopy; CARBON-DIOXIDE; RHODIUM; CONVERSION; OXIDATION; ALUMINA; ENERGY; RH;
D O I
10.1016/j.cattod.2010.06.016
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Experimental evidences show that it is possible to produce methane from an exclusively inorganic way using CO2 and H-2 on a Rh/gamma-Al2O3 catalyst at low temperature and atmospheric pressure New insights on the mechanism of methanation are given The first step of the mechanism in the methanation reaction could be the chemisorption of CO2 on the catalyst The second step is the dissociation of CO2 into CO and O adsorbed on the surface The third step is the reaction of dissociated species with H-2 Adsorption dissociation of CO2 and the reaction of dissociated species with H-2 are evidenced by in situ DRIFT experiments The reaction could occur between the adsorbed species However a reaction between adsorbed species and gaseous hydrogen cannot be excluded XPS shows that the CO2 oxidizes the catalyst and this oxidation deactivates the catalyst The conversion of CO2 also increases with temperature Methane is the unique hydrocarbon molecule formed and obtained with almost 100% selectivity No other hydrocarbonated products have been observed (C) 2010 Elsevier B V All rights reserved
引用
收藏
页码:462 / 466
页数:5
相关论文
共 21 条
  • [1] ALONSO FJP, 2008, CATAL COMMUN, V9, P1945
  • [2] The contribution of the utilization option to reducing the CO2 atmospheric loading:: research needed to overcome existing barriers for a full exploitation of the potential of the CO2 use
    Aresta, M
    Dibenedetto, A
    [J]. CATALYSIS TODAY, 2004, 98 (04) : 455 - 462
  • [3] Selective conversion of ethylbenzene into styrene over K2O/TiO2-ZrO2 catalysts:: Unified effects of K2O and CO2
    Burri, David Raju
    Choi, Kwang-Min
    Han, Sang-Cheol
    Burri, Abhishek
    Park, Sang-Eon
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2007, 269 (1-2) : 58 - 63
  • [4] Influence of the co-feeding of CO, H2, CO2 or H2O in the partial oxidation of methane over Ni and Rh supported catalysts
    Cellier, C
    Le Clef, D
    Mateos-Pedrero, C
    Ruiz, P
    [J]. CATALYSIS TODAY, 2005, 106 (1-4) : 47 - 51
  • [5] Nickel supported on rice husk ash -: activity and selectivity in CO2 methanation
    Chang, FW
    Hsiao, TJ
    Chung, SW
    Lo, JJ
    [J]. APPLIED CATALYSIS A-GENERAL, 1997, 164 (1-2) : 225 - 236
  • [6] DUBOIS LH, 1983, SURF SCI, V128, pL231, DOI 10.1016/S0039-6028(83)80009-0
  • [7] EFFECT OF PARTIAL REDUCTION ON THE FORMATION OF OXYGENATED COMPOUNDS IN THE HYDROGENATION OF CARBON-MONOXIDE ON RHODIUM ALUMINA
    DUPREZ, D
    BARRAULT, J
    GERON, C
    [J]. APPLIED CATALYSIS, 1988, 37 (1-2): : 105 - 114
  • [8] The active role of CO2 at low temperature in oxidation processes:: the case of the oxidative dehydrogenation of propane on NiMoO4 catalysts
    Dury, F
    Gaigneaux, EM
    Ruiz, P
    [J]. APPLIED CATALYSIS A-GENERAL, 2003, 242 (01) : 187 - 203
  • [9] GRATZEL M, 1989, Patent No. 4847231
  • [10] Alkali-metal promoted rhodium-on-alumina catalysts for nitrous oxide decomposition
    Haber, Jerzy
    Nattich, Malgorzata
    Machej, Tadeusz
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 77 (3-4) : 278 - 283