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

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Science  14 May 2004:
Vol. 304, Issue 5673, pp. 992-995
DOI: 10.1126/science.1096309

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State-resolved gas-surface reactivity measurements revealed that vibrational excitation of ν3 (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 ν3 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.

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