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Volume 157, 2012
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Vibrationally bond-selected chemisorption of methane isotopologues on Pt(111) studied by reflection absorption infrared spectroscopy

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Abstract

Reflection absorption infrared spectroscopy (RAIRS) was used to probe for vibrational bond-selectivity in the dissociative chemisorption of three partially deuterated methane isotopologues on a Pt(111) surface. While a combination of incident translational energy and thermal vibrational excitation produces a nearly statistical distribution of C–H and C–D bond cleavage products, we observe that laser excitation of an infrared active C–H stretch normal mode leads to highly selective dissociation of a C–H bond for CHD3, CH2D2, and CH3D. Our results show that vibrational energy redistribution between C–H and C–D stretch modes due to methane/surface interactions is negligible during the sub-picosecond collision time which indicates that vibrational bond-selectivity may be the rule rather than the exception in heterogeneous reactions of small polyatomic molecules.

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Publication details

The article was received on 18 Jan 2012, accepted on 14 Feb 2012 and first published on 15 Feb 2012


Article type: Paper
DOI: 10.1039/C2FD20007D
Citation: Faraday Discuss., 2012,157, 285-295
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    Vibrationally bond-selected chemisorption of methane isotopologues on Pt(111) studied by reflection absorption infrared spectroscopy

    L. Chen, H. Ueta, R. Bisson and R. D. Beck, Faraday Discuss., 2012, 157, 285
    DOI: 10.1039/C2FD20007D

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