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Journal of Chemical Physics / Volume 136 / Issue 6 / COMMUNICATIONS
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J. Chem. Phys. 136, 061101 (2012); http://dx.doi.org/10.1063/1.3685833 (4 pages)

Communication: Angle-resolved thermal dissociative sticking of CH4 on Pt(111): Further indication that rotation is a spectator to the gas-surface reaction dynamics

J. K. Navin, S. B. Donald, D. G. Tinney, G. W. Cushing, and I. Harrison

Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904-4319, USA

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(Received 21 December 2011; accepted 30 January 2012; published online 9 February 2012)

Effusive molecular beam measurements of angle-resolved thermal dissociative sticking coefficients for CH4 impinging on a Pt(111) surface, at a temperature of 700 K, are reported and compared to theoretical predictions. The reactivity falls off steeply as the molecular angle of incidence increases away from the surface normal. Successful modeling of the thermal dissociative sticking behavior, consistent with existent CH4 supersonic molecular beam experiments involving rotationally cold molecules, required that rotation be treated as a spectator degree of freedom.

© 2012 American Institute of Physics

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KEYWORDS and PACS

Keywords

adsorption, dissociation, molecular beams, organic compounds, platinum

PACS

  • 68.43.Mn

    Adsorption kinetics

  • 82.30.Lp

    Decomposition reactions (pyrolysis, dissociation, and fragmentation)

  • 37.20.+j

    Atomic and molecular beam sources and techniques

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3685833

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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Figures (1) Tables (1)

Figures (click on thumbnails to view enlargements)

FIG.1
Effusive molecular beam measurements of the CH4/Pt(111) angle-resolved thermal dissociative sticking coefficient at 700 K (open points) are compared to angular distribution predictions (lines) from several theoretical models whose parameters15 were optimized to a limited set of supersonic molecular beam experiments10 performed at a nozzle temperature of 680 K and 300 K. The parameters and S(700 K, ϑ) predictions of the models are given in Table 1. The S(700 K, ϑ) predictions scaled by the divisors yielding the best fits to the experimental data appear as the lines of this figure.

FIG.1 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

Tables

Table I. CH4/Pt(111) angle-resolved thermal dissociative sticking coefficient.

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