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
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