Semi-Empirical Calculations on the Stability and Reactivity of NHx Species on Metal Surfaces Full article
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Catalysis Letters
ISSN: 1011-372X , E-ISSN: 1572-879X |
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| Output data | Year: 2003, Volume: 86, Number: 1-3, Pages: 9-16 Pages count : 8 DOI: 10.1023/A:1022607008230 | ||||
| Tags | NHx intermediates, NO + H2 reaction, Noble metals, Oscillation phenomena, Semi-empirical calculations, Single-crystal surfaces | ||||
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| Affiliations |
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Funding (1)
| 1 | International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union | 99-01882 |
Abstract:
The semi-empirical method of interacting bonds was used to elucidate the mechanism of oscillation phenomena in the NO + H2 reaction on metal surfaces. Basic single-crystal planes of Pt, Rh, Ir, Fe, Ru, and Re were examined with respect to the stability of adsorbed NHn species (n = 0, 1, 2, 3); to the reactivity of NHn (n = 0, 1, 2) species toward adsorbed hydrogen atoms; and to the possibility of combination reactions between two NH or two NH2 species resulting in the formation of gaseous N2 molecules. All studied surfaces were found to form readily stable NH species. The principal difference between Pt, Rh, and Ir single-crystal planes exhibiting reaction rate oscillations, and Fe, Ru, and Re surfaces, which do not show an oscillatory behavior, is that the combination reaction of NH species can easily proceed in the former case, whereas this reaction is not allowed thermodynamically in the latter. This result is consistent with an earlier suggested model that attributes the oscillatory surface wave propagation to the intermediate formation of NH species.
Stable NH2 species can be formed on Ru, Re, and Fe surfaces, whereas the noble metal surfaces of Pt, Rh, and Ir can only form weakly stable NH2 species at the very edge of their existence region. The combination reaction between two NH2 species is endothermic in all cases.
Cite:
Cholach A.R.
, Bulgakov N.N.
, Nieuwenhuys B.E.
Semi-Empirical Calculations on the Stability and Reactivity of NHx Species on Metal Surfaces
Catalysis Letters. 2003. V.86. N1-3. P.9-16. DOI: 10.1023/A:1022607008230 WOS Scopus РИНЦ ANCAN OpenAlex
Semi-Empirical Calculations on the Stability and Reactivity of NHx Species on Metal Surfaces
Catalysis Letters. 2003. V.86. N1-3. P.9-16. DOI: 10.1023/A:1022607008230 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
| Submitted: | Sep 19, 2002 |
| Accepted: | Nov 13, 2002 |
| Published print: | Mar 1, 2003 |
Identifiers:
| Web of science: | WOS:000181044100002 |
| Scopus: | 2-s2.0-0037367642 |
| Elibrary: | 13425146 |
| Chemical Abstracts: | 2003:125805 |
| Chemical Abstracts (print): | 138:407469 |
| OpenAlex: | W334633221 |