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Adsorption and dissociation of NO on stepped Pt(533)
被引:41
作者:
Backus, EHG
Eichler, A
Grecea, ML
Kleyn, AW
Bonn, M
机构:
[1] Leiden Univ, Leiden Inst Chem, NL-2300 RA Leiden, Netherlands
[2] Univ Vienna, Inst Mat Phys, A-1090 Vienna, Austria
[3] Univ Vienna, Ctr Computat Mat Sci, A-1090 Vienna, Austria
[4] EURATOM FOM Associat, FOM Inst Plasma Phys Rijnhuizen, NL-3430 BE Nieuwegein, Netherlands
[5] FOM, Inst Atom & Mol Phys, NL-1098 SJ Amsterdam, Netherlands
关键词:
D O I:
10.1063/1.1799956
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:
We present an experimental and theoretical investigation of the adsorption, desorption, and dissociation of NO on the stepped Pt (533) surface. By combining temperature programmed desorption and reflection absorption infrared spectroscopy, information about the adsorption sites at different temperatures is obtained. Surprisingly, metastable adsorption structures of NO can be produced through variation of the dosing temperature. We also show that part of the NO molecules adsorbed on the step sites dissociates around 450 K. After dissociation the N atoms can desorb either by combining with an O fragment, or with another N atom, resulting in NO and N-2. The N-2 production can be enhanced by coadsorbing CO on the surface: CO scavenges the oxygen atom, thereby suppressing associative recombinative desorption of N and O atoms. Density functional theory calculations are used to reveal the adsorption energies and vibrational frequencies of adsorbed NO as well as barriers for dissociation of NO and for diffusion of N atoms. The combined experimental results and theoretical calculations reveal that dissociation of NO is the rate limiting step in the formation of N-2. (C) 2004 American Institute of Physics.
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页码:7946 / 7954
页数:9
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