CO2 Hydrogenation to Methanol on Supported Au Catalysts under Moderate Reaction Conditions: Support and Particle Size Effects

被引:141
作者
Hartadi, Yeusy [1 ]
Widmann, Daniel [1 ]
Behm, R. Juergen [1 ]
机构
[1] Univ Ulm, Inst Surface Chem & Catalysis, D-89081 Ulm, Germany
关键词
hydrogenation; kinetics; gold; supported catalysts; renewable resources; GAS SHIFT REACTION; GOLD CATALYSTS; CARBON-DIOXIDE; AU/TIO2; CATALYSTS; AU/CEO2; CATALYST; OXIDE SURFACES; ACTIVE-SITES; METAL-OXIDES; OXIDATION; OXYGEN;
D O I
10.1002/cssc.201402645
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The potential of metal oxide supported Au catalysts for the formation of methanol from CO2 and H-2 under conditions favorable for decentralized and local conversion, which could be concepts for chemical energy storage, was investigated. Significant differences in the catalytic activity and selectivity of Au/Al2O3, Au/TiO2, AuZnO, and Au/ZrO2 catalysts for methanol formation under moderate reaction conditions at a pressure of 5bar and temperatures between 220 and 240 degrees C demonstrate pronounced support effects. A high selectivity (>50%) for methanol formation was obtained only for Au/ZnO. Furthermore, measurements on Au/ZnO samples with different Au particle sizes reveal distinct Au particle size effects: although the activity increases strongly with the decreasing particle size, the selectivity decreases. The consequences of these findings for the reaction mechanism and for the potential of Au/ZnO catalysts for chemical energy storage and a green methanol technology are discussed.
引用
收藏
页码:456 / 465
页数:10
相关论文
共 55 条
  • [11] Chemoselective hydrogenation of nitro compounds with supported gold catalysts
    Corma, Avelino
    Serna, Pedro
    [J]. SCIENCE, 2006, 313 (5785) : 332 - 334
  • [12] Activity, stability, and deactivation behavior of supported Au/TiO2 catalysts in the CO oxidation and preferential CO oxidation reaction at elevated temperatures
    Denkwitz, Yvonne
    Schumacher, Birgit
    Kucerova, Gabriela
    Behm, R. Juergen
    [J]. JOURNAL OF CATALYSIS, 2009, 267 (01) : 78 - 88
  • [13] Why hybrid porous solids capture greenhouse gases?
    Ferey, Gerard
    Serre, Christian
    Devic, Thomas
    Maurin, Guillaume
    Jobic, Herve
    Llewellyn, Philip L.
    De Weireld, Guy
    Vimont, Alexandre
    Daturi, Marco
    Chang, Jong-San
    [J]. CHEMICAL SOCIETY REVIEWS, 2011, 40 (02) : 550 - 562
  • [14] Föttinger K, 2013, SPR-CATAL, V25, P77, DOI 10.1039/9781849737203-00077
  • [15] Identification and characterization of active sites and their catalytic processes - the Cu/ZnO methanol catalyst
    French, SA
    Sokol, AA
    Bromley, ST
    Catlow, CRA
    Sherwood, P
    [J]. TOPICS IN CATALYSIS, 2003, 24 (1-4) : 161 - 172
  • [16] French SA, 2001, ANGEW CHEM INT EDIT, V40, P4437, DOI 10.1002/1521-3773(20011203)40:23<4437::AID-ANIE4437>3.0.CO
  • [17] 2-L
  • [18] JUNCTION EFFECT INTERACTIONS IN METHANOL SYNTHESIS CATALYSTS
    FROST, JC
    [J]. NATURE, 1988, 334 (6183) : 577 - 580
  • [19] Gold-ceria catalysts for low-temperature water-gas shift reaction
    Fu, Q
    Kudriavtseva, S
    Saltsburg, H
    Flytzani-Stephanopoulos, M
    [J]. CHEMICAL ENGINEERING JOURNAL, 2003, 93 (01) : 41 - 53
  • [20] The kinetics and mechanism of methanol synthesis by hydrogenation of CO2 over a Zn-deposited Cu(111) surface
    Fujitani, T
    Nakamura, I
    Uchijima, T
    Nakamura, J
    [J]. SURFACE SCIENCE, 1997, 383 (2-3) : 285 - 298