KINETICS OF THE COMPLETE OXIDATION OF METHANE OVER SUPPORTED PALLADIUM CATALYSTS

被引:382
作者
RIBEIRO, FH [1 ]
CHOW, M [1 ]
DALLABETTA, RA [1 ]
机构
[1] CATALYT INC,430 FERGUSON DR,BLDG 3,MT VIEW,CA 94043
关键词
D O I
10.1006/jcat.1994.1092
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
The complete oxidation of methane by supported Pd was studied in a reaction mixture of 2% CH4 in air at 550 K, and atmospheric pressure. The catalysts were Pd supported on Al2O3 and ZrO2 deposited from PdCl2 or Pd(NH3)2(NO2)2 precursors. For the determination of how the turnover rate varies with the structure of the catalyst, the average Pd particle size on the series of catalysts was varied in the critical size range (1-10 nm). The number of active sites were measured before and after reaction by the method of H2 titration of adsorbed oxygen at 373 K. The number of active sites remained the same, although the rate per gram of catalyst increased with time on stream for all catalysts. At steady-state, the turnover rate for the series of catalysts tested varied in the range 2 x 10(-2) to 8 x 10(-2) S-1 under the conditions of these experiments. It is concluded that the reaction is structure insensitive. In an investigation of the kinetics of methane oxidation on palladium, the reaction products were found to strongly inhibit the oxidation of methane. (C) 1994 Academic Press, Inc.
引用
收藏
页码:537 / 544
页数:8
相关论文
共 32 条
  • [1] Anderson JR, 1975, STRUCTURE METALLIC C, P296
  • [2] CATALYTIC OXIDATION OF METHANE
    ANDERSON, RB
    STEIN, KC
    FEENAN, JJ
    HOFER, LJE
    [J]. INDUSTRIAL AND ENGINEERING CHEMISTRY, 1961, 53 (10): : 809 - 812
  • [3] REMARKABLE ACTIVITY ENHANCEMENT IN THE CATALYTIC COMBUSTION OF METHANE ON SUPPORTED PALLADIUM CATALYSTS
    BALDWIN, TR
    BURCH, R
    [J]. CATALYSIS LETTERS, 1990, 6 (01) : 131 - 138
  • [4] CATALYTIC COMBUSTION OF METHANE OVER SUPPORTED PALLADIUM CATALYSTS .1. ALUMINA SUPPORTED CATALYSTS
    BALDWIN, TR
    BURCH, R
    [J]. APPLIED CATALYSIS, 1990, 66 (02): : 337 - 358
  • [5] HYDROGEN-OXYGEN TITRATION METHOD FOR MEASUREMENT OF SUPPORTED PALLADIUM SURFACE-AREAS
    BENSON, JE
    HWANG, HS
    BOUDART, M
    [J]. JOURNAL OF CATALYSIS, 1973, 30 (01) : 146 - 153
  • [6] SOLUBILITY OF HYDROGEN IN SMALL PARTICLES OF PALLADIUM
    BOUDART, M
    HWANG, HS
    [J]. JOURNAL OF CATALYSIS, 1975, 39 (01) : 44 - 52
  • [7] Boudart M., 1984, KINETICS HETEROGENEO, P118
  • [8] BRILL R, 1969, C INT CNRS, V187, P99
  • [9] EFFECT OF PARTICLE-SIZE ON THE REACTIVITY OF OXYGEN-ADSORBED PLATINUM SUPPORTED ON ALUMINA
    BRIOT, P
    AUROUX, A
    JONES, D
    PRIMET, M
    [J]. APPLIED CATALYSIS, 1990, 59 (01): : 141 - 152
  • [10] CATALYTIC-OXIDATION OF METHANE OVER PALLADIUM SUPPORTED ON ALUMINA - EFFECT OF AGING UNDER REACTANTS
    BRIOT, P
    PRIMET, M
    [J]. APPLIED CATALYSIS, 1991, 68 (1-2): : 301 - 314