Selective catalytic oxidation of CO: Effect of chloride on supported Au catalysts

被引:210
作者
Oh, HS
Yang, JH
Costello, CK
Wang, YM
Bare, SR
Kung, HH [1 ]
Kung, MC
机构
[1] Northwestern Univ, Dept Chem Engn, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Mat Sci, Evanston, IL 60208 USA
[3] UOP Res Ctr, Des Plaines, IL 60017 USA
基金
美国国家科学基金会;
关键词
chloride; gold; poisoning; selective CO oxidation;
D O I
10.1006/jcat.2002.3710
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
Supported Au catalysts are generally prepared from chloride-containing An precursors and their properties are highly sensitive to preparation procedures. To better understand and control the variables important in the preparation of these catalysts, the effect of chloride on the catalytic performances of highly active Au/Al2O3 catalysts in the selective catalytic oxidation of CO (SCO) was probed. The complex manner in which Cl- affected An catalysis was deconvoluted in a series of complementary experiments where chloride was quantitatively removed and added. The residual chloride was found to affect the activities in two different ways. It facilitates the agglomeration of An particles during heat treatment, and it inhibits the catalytic activity by poisoning the active site. Interestingly, chloride poisoning is not only observed at the steady state, it is in fact more pronounced in the transient toward steady state. In order to better assess the poisoning effect of Cl-, phosphate was introduced to the support surface as a postsynthesis treatment before the addition of Cl- in some experiments. The results showed that activity suppression was observable at a Cl-/Au molar ratio as low as 0.0006. Thus a very small fraction of Au is associated with the active site. This implies that the activity per active site is extremely high. (C) 2002 Elsevier Science (USA).
引用
收藏
页码:375 / 386
页数:12
相关论文
共 25 条
  • [1] Low-temperature water-gas shift reaction on Au/alpha-Fe2O3 catalyst
    Andreeva, D
    Idakiev, V
    Tabakova, T
    Andreev, A
    Giovanoli, R
    [J]. APPLIED CATALYSIS A-GENERAL, 1996, 134 (02) : 275 - 283
  • [2] BATES CF, 1976, HYDROLYSIS CATIONS
  • [3] BETHKE GK, 2000, APPL CATAL A-GEN, V43, P194
  • [4] Supported Ag catalysts for the lean reduction of NO with C3H6
    Bethke, KA
    Kung, HH
    [J]. JOURNAL OF CATALYSIS, 1997, 172 (01) : 93 - 102
  • [5] 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
  • [6] Gold-catalysed oxidation of carbon monoxide
    Bond, GC
    Thompson, DT
    [J]. GOLD BULLETIN, 2000, 33 (02) : 41 - 51
  • [7] CHE M, 1993, P 10 INT C CAT BUD 1, P32
  • [8] Nature of the active site for CO oxidation on highly active Au/γ-Al2O3
    Costello, CK
    Kung, MC
    Oh, HS
    Wang, Y
    Kung, HH
    [J]. APPLIED CATALYSIS A-GENERAL, 2002, 232 (1-2) : 159 - 168
  • [9] LOW-TEMPERATURE OXIDATION OF CO OVER GOLD SUPPORTED ON TIO2, ALPHA-FE2O3, AND CO3O4
    HARUTA, M
    TSUBOTA, S
    KOBAYASHI, T
    KAGEYAMA, H
    GENET, MJ
    DELMON, B
    [J]. JOURNAL OF CATALYSIS, 1993, 144 (01) : 175 - 192
  • [10] Size- and support-dependency in the catalysis of gold
    Haruta, M
    [J]. CATALYSIS TODAY, 1997, 36 (01) : 153 - 166