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Science 14 May 2004:
Vol. 304. no. 5673, pp. 992 - 995
DOI: 10.1126/science.1096309
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Reports

Preference for Vibrational over Translational Energy in a Gas-Surface Reaction

R. R. Smith, D. R. Killelea, D. F. DelSesto, A. L. Utz

State-resolved gas-surface reactivity measurements revealed that vibrational excitation of {nu}3 (the antisymmetric C-H stretch) activates methane dissociation more efficiently than does translational energy. Methane molecules in the vibrational ground state require 45 kilojoules per mole (kJ/mol) of translational energy to attain the same reactivity enhancement provided by 36 kJ/mol of {nu}3 excitation. This result contradicts a key assumption underlying statistical theories of gas-surface reactivity and provides direct experimental evidence of the central role that vibrational energy can play in activating gas-surface reactions.

Department of Chemistry and W. M. Keck Foundation Laboratory for Materials Chemistry, Tufts University, Medford, MA 02155, USA.

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THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Chemical Dynamics Special Feature: Vibrational vs. translational energy in promoting a prototype metal-hydrocarbon insertion reaction.
D. L. Proctor and H. F. Davis (2008)
PNAS 105, 12673-12677
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Chemical Dynamics Special Feature: Chemical dynamics of vibrationally excited molecules: Controlling reactions in gases and on surfaces.
F. F. Crim (2008)
PNAS 105, 12654-12661
   Abstract »    Full Text »    PDF »
Bond-Selective Control of a Heterogeneously Catalyzed Reaction.
D. R. Killelea, V. L. Campbell, N. S. Shuman, and A. L. Utz (2008)
Science 319, 790-793
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Science. ISSN 0036-8075 (print), 1095-9203 (online)