Mode-specific reactivity of CH4 on Pt(110)-(1 x 2) : The concerted role of stretch and bend excitation

Bisson, R, Sacchi, M and Beck, RD (2010) Mode-specific reactivity of CH4 on Pt(110)-(1 x 2) : The concerted role of stretch and bend excitation Physical Review B, 82.

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Abstract

The state-resolved reaction probability of CH4 on Pt(110)−(1×2) was measured as a function of CH4 translational energy for four vibrational eigenstates comprising different amounts of C-H stretch and bend excitation. Mode-specific reactivity is observed both between states from different polyads and between isoenergetic states belonging to the same polyad of CH4. For the stretch/bend combination states, the vibrational efficacy of reaction activation is observed to be higher than for either pure C-H stretching or pure bending states, demonstrating a concerted role of stretch and bend excitation in C-H bond scission. This concerted role, reflected by the nonadditivity of the vibrational efficacies, is consistent with transition state structures found by ab initio calculations and indicates that current dynamical models of CH4 chemisorption neglect an important degree of freedom by including only C-H stretching motion.

Item Type:	Article
Subjects :	Chemistry
Authors :	Name Email ORCID Bisson, R Sacchi, M m.sacchi@surrey.ac.uk Beck, RD
Date :	9 September 2010
DOI :	10.1103/PhysRevB.82.121404
Copyright Disclaimer :	© 2010 The American Physical Society
Depositing User :	Symplectic Elements
Date Deposited :	17 May 2017 13:56
Last Modified :	16 Jan 2019 18:51
URI:	http://epubs.surrey.ac.uk/id/eprint/840866

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