Oscillatory behaviour in the NO-H2 reaction over Ir(510)

被引:9
作者
de Wolf, CA [1 ]
Hattink, MO [1 ]
Nieuwenhuys, BE [1 ]
机构
[1] Leiden Univ, Leiden Inst Chem, NL-2300 RA Leiden, Netherlands
关键词
models of non-linear phenomena; catalysis; iridium; hydrogen molecule; nitrogen oxides; stepped single crystal surfaces;
D O I
10.1016/S0039-6028(00)00900-6
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 non-linear behaviour in the NO-H-2 reaction over the stepped Ir(5 1 0) was studied using mass spectrometry, LEED and AES with NO pressures between 7.7 x 10(-8) and 7.7 x 10(-7) mbar and H-2/NO ratios ranging from 1 to 54. In addition. TDS experiments were carried out to study the interaction between the species present on the surface during the reaction. During temperature programmed heating of a NO saturated surface in the presence of a hydrogen flow an explosive formation of N-2. and to a lesser extent H2O, was observed, indicative of an autocatalytic reaction. Furthermore. TDS experiments on a NO saturated surface that was precovered with O, showed that the presence of O-ads lowers the NO activation energy of desorption by 12 kJ mol(-1) During a heating-cooling cycle an adsorbate induced lifting of the surface reconstruction was observed under similar reaction conditions at which oscillations in rate were observed. The rates of N and H2O formation are in-phase during these oscillations. No other products were observed under oscillatory conditions. Possible mechanisms of the oscillations are discussed. Finally. a comparison between the non-linear behaviour over Ir(5 1 0), Pt(1 0 0) and other Ir and Ph surfaces was made. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:114 / 124
页数:11
相关论文
共 56 条
[21]   INTERACTION OF O-2 WITH PT(100) .1. EQUILIBRIUM MEASUREMENTS [J].
GRIFFITHS, K ;
JACKMAN, TE ;
DAVIES, JA ;
NORTON, PR .
SURFACE SCIENCE, 1984, 138 (01) :113-124
[22]   Simulation of oscillatory behaviour in the reduction of NO by hydrogen on Pt{100}: The role of non-linear restructuring [J].
Gruyters, M ;
Pasteur, AT ;
King, DA .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (16) :2941-2949
[23]   SURFACE STRUCTURES ON CLEAN PLATINUM (100) SURFACE [J].
HAGSTROM, S ;
LYON, HB ;
SOMORJAI, GA .
PHYSICAL REVIEW LETTERS, 1965, 15 (11) :491-&
[24]   DYNAMICS OF THE RECONSTRUCTION PROCESS IR(100)1X1-]1X5 [J].
HEINZ, K ;
SCHMIDT, G ;
HAMMER, L ;
MULLER, K .
PHYSICAL REVIEW B, 1985, 32 (10) :6214-6221
[25]   LEED INVESTIGATIONS OF XENON SINGLE-CRYSTAL FILMS AND THEIR USE IN STUDYING IR(100) SURFACE [J].
IGNATIEV, A ;
JONES, AV ;
RHODIN, TN .
SURFACE SCIENCE, 1972, 30 (03) :573-&
[26]   OSCILLATORY KINETICS IN HETEROGENEOUS CATALYSIS [J].
IMBIHL, R ;
ERTL, G .
CHEMICAL REVIEWS, 1995, 95 (03) :697-733
[27]   OSCILLATORY REACTIONS ON SINGLE-CRYSTAL SURFACES [J].
IMBIHL, R .
PROGRESS IN SURFACE SCIENCE, 1993, 44 (3-4) :185-343
[28]   Structure and phase behavior of the Ir(001) surface: X-ray scattering measurements [J].
Jahns, V ;
Zehner, DM ;
Watson, GM ;
Gibbs, D .
SURFACE SCIENCE, 1999, 430 (1-3) :55-66
[29]   HYSTERESIS AND OSCILLATIONS IN THE SELECTIVITY DURING THE NO-H-2 REACTION OVER RH(533) [J].
JANSSEN, NMH ;
COBDEN, PD ;
NIEUWENHUYS, BE ;
IKAI, M ;
MUKAI, K ;
TANAKA, K .
CATALYSIS LETTERS, 1995, 35 (1-2) :155-163
[30]   OSCILLATORY BEHAVIOR OF THE NO-H-2 REACTION OVER RH(533) [J].
JANSSEN, NMH ;
NIEUWENHUYS, BE ;
IKAI, M ;
TANAKA, K ;
CHOLACH, AR .
SURFACE SCIENCE, 1994, 319 (03) :L29-L33