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  The mechanism of the “explosive” NO + CO reaction on Pt(100): experiments and mathematical modeling

Fink, T., Dath, J. P., Basset, M. R., Imbihl, R., & Ertl, G. (1991). The mechanism of the “explosive” NO + CO reaction on Pt(100): experiments and mathematical modeling. Surface Science, 245(1-2), 96-110. doi:10.1016/0039-6028(91)90471-4.

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 Creators:
Fink, Th.1, Author           
Dath, J. P.2, Author
Basset, M. R.3, Author
Imbihl, Ronald4, Author           
Ertl, Gerhard4, Author           
Affiliations:
1Fritz Haber Institute, Max Planck Society, ou_24021              
2Universite de l’Etat a Mons, Laboratoire de Chimie Inorganique et Analytique , 23 Avenue Maistriau, B-7000 Mans, Belgium., ou_persistent22              
3Union Carbide Corporation, P.O. Box 8361, South Charleston, WV 25303, USA. , ou_persistent22              
4Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              

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 Abstract: Coadsorbed NO and CO on a Pt(100) surface react upon heating to form extremely narrow TPR product peaks of CO2 and N2 at ~ 400 K whose position and half-width are almost independent of the initial coverages. Video-LEED, TDS and work-function measurements were used to study the adsorption behavior of NO and the surface reaction between coadsorbed NO and CO. The LEED experiments demonstrated that at higher coverages the “explosive” formation of CO2 and N2 is not accompanied by the 1 × 1 → hex phase transition which is shifted up by ~ 50 K to higher temperature. This result rules out the phase transition as a possible explanation for the narrowness of the product peaks in TPR. A new model is proposed based on the vacant site requirement for NO dissociation in which the autocatalytic increase in the number of vacant sites during the surface reaction is responsible for the ‘surface explosion”. This simple vacancy model is modified by taking island formation into account in order to reproduce the coverage independent position and shape of the product peaks. Island formation occurs in the NO/CO-induced lifting of the hex reconstruction as a consequence of the higher adsorption energy of NO/CO on the 1 × 1 phase. Based on these mechanistic steps a mathematical model was developed consisting of five coupled differential equations whose solutions reproduce the experimental results quite accurately.

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Language(s): eng - English
 Dates: 1990-08-021990-10-261991-04-01
 Publication Status: Issued
 Pages: 15
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/0039-6028(91)90471-4
 Degree: -

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Title: Surface Science
  Abbreviation : Surf. Sci.
Source Genre: Journal
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Publ. Info: Amsterdam : Elsevier
Pages: 15 Volume / Issue: 245 (1-2) Sequence Number: - Start / End Page: 96 - 110 Identifier: ISSN: 0039-6028
CoNE: https://pure.mpg.de/cone/journals/resource/0039-6028