Au/MgO catalysts modified with ascorbic acid for low temperature CO oxidation

被引:102
作者
Margitfalvi, JL
Fási, A
Hegedus, M
Lónyi, F
Gobölös, S
Bogdanchikova, N
机构
[1] Hungarian Acad Sci, Inst Chem, Chem Res Ctr, H-1025 Budapest, Hungary
[2] Univ Nacl Autonoma Mexico, Ctr Ciencias Mat Condensada, Ensenada, Baja California, Mexico
关键词
Au/MgO catalyst; CO oxidation; low temperature oxidation; catalyst modification; ascorbic acid;
D O I
10.1016/S0920-5861(01)00489-8
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Au/Mg(OH)(2) catalyst was modified with different amounts of ascorbic acid. After dehydration at 350degreesC, in various atmospheres, the modified Au/MgO catalysts were characterized and tested in the oxidation of CO. It has been shown for the first time that at high CO pressure supported gold chemisorbs CO and the apparent gold dispersion can be determined. The oxidation of CO was investigated in the temperature range between -30 and 250 degreesC using both temperature-programmed oxidation technique and time on stream experiments. A characteristic feature of Au/MgO catalysts is the decrease of the activity upon increasing the reaction temperature from -30 to 110-120 degreesC. The results showed that the introduction of ascorbic acid had a definite positive effect on the activity of Au/MgO catalyst in low temperature CO oxidation. This effect strongly depended on the amount of ascorbic acid introduced and had a distinct optimum. Based on diffuse reflection UV-VIS and in situ FTIR spectroscopic data it is suggested that the addition of ascorbic acid (i) slightly alters the (ionic gold)/(metallic gold) ratio in both the parent (Au/Mg(OH)(2)) and the working catalysts (Au/MgO) and (ii) suppresses the carbonate formation responsible for the deactivation, It is proposed that the activation of CO requires the formation of "(Audelta+)(m)-Au-n" ensemble sites, in which the ionic gold is involved in the activation of CO molecule via Audelta+-carbonyl oxygen interaction. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:157 / 169
页数:13
相关论文
共 22 条
  • [1] CHEMICAL REACTIVITY OF SUPPORTED GOLD .3. ATOMIC BINDING AND COORDINATION OF GOLD FROM X-RAY ABSORPTION FINE-STRUCTURE SPECTROSCOPY
    BASSI, IW
    LYTLE, FW
    PARRAVANO, G
    [J]. JOURNAL OF CATALYSIS, 1976, 42 (01) : 139 - 147
  • [2] FTIR study of the low-temperature water-gas shift reaction on Au/Fe2O3 and Au/TiO2 catalysts
    Boccuzzi, F
    Chiorino, A
    Manzoli, M
    Andreeva, D
    Tabakova, T
    [J]. JOURNAL OF CATALYSIS, 1999, 188 (01) : 176 - 185
  • [3] A kinetic and DRIFTS study of low-temperature carbon monoxide oxidation over Au-TiO2 catalysts
    Bollinger, MA
    Vannice, MA
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 8 (04) : 417 - 443
  • [4] Structural analysis of Au/TiO2 catalysts by Debye function analysis
    Cunningham, DAH
    Vogel, W
    Sanchez, RMT
    Tanaka, K
    Haruta, M
    [J]. JOURNAL OF CATALYSIS, 1999, 183 (01) : 24 - 31
  • [5] The relationship between the structure and activity of nanometer size gold when supported on Mg(OH)2
    Cunningham, DAH
    Vogel, W
    Kageyama, H
    Tsubota, S
    Haruta, M
    [J]. JOURNAL OF CATALYSIS, 1998, 177 (01) : 1 - 10
  • [6] Negative activation energies in CO oxidation over an icosahedral Au/Mg(OH)2 catalyst
    Cunningham, DAH
    Vogel, W
    Haruta, M
    [J]. CATALYSIS LETTERS, 1999, 63 (1-2) : 43 - 47
  • [7] ELLIOT GS, 1984, P 14 INT S RAR GAS D, V1, P349
  • [8] CHEMICAL REACTIVITY OF SUPPORTED GOLD .4. REDUCTION OF NO BY H-2
    GALVAGNO, S
    PARRAVANO, G
    [J]. JOURNAL OF CATALYSIS, 1978, 55 (02) : 178 - 190
  • [9] Selective oxidation of CO over supported Au catalysts
    Grisel, RJH
    Nieuwenhuys, BE
    [J]. JOURNAL OF CATALYSIS, 2001, 199 (01) : 48 - 59
  • [10] Preparation of supported gold catalysts for low-temperature CO oxidation via "size-controlled" gold colloids
    Grunwaldt, JD
    Kiener, C
    Wögerbauer, C
    Baiker, A
    [J]. JOURNAL OF CATALYSIS, 1999, 181 (02) : 223 - 232