Vibrationally Promoted Dissociation of Water on Ni(111)

Water dissociation on transition-metal catalysts is an important step in steam reforming and the water-gas shift reaction. To probe the effect of translational and vibrational activation on this important heterogeneous reaction, we performed state-resolved gas/surface reactivity measurements for the...

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Veröffentlicht in:Science (American Association for the Advancement of Science) 2014-05, Vol.344 (6183), p.504-507
Hauptverfasser: Hundt, P. Morten, Jiang, Bin, van Reijzen, Maarten E., Guo, Hua, Beck, Rainer D.
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container_end_page 507
container_issue 6183
container_start_page 504
container_title Science (American Association for the Advancement of Science)
container_volume 344
creator Hundt, P. Morten
Jiang, Bin
van Reijzen, Maarten E.
Guo, Hua
Beck, Rainer D.
description Water dissociation on transition-metal catalysts is an important step in steam reforming and the water-gas shift reaction. To probe the effect of translational and vibrational activation on this important heterogeneous reaction, we performed state-resolved gas/surface reactivity measurements for the dissociative chemisorption of D2O on Ni(111), using molecular beam techniques. The reaction occurs via a direct pathway, because both the translational and vibrational energies promote the dissociation. The experimentally measured initial sticking probabilities were used to calibrate a first-principles potential energy surface based on density functional theory. Quantum dynamical calculations on the scaled potential energy surface reproduced the experimental results semiquantitatively. The larger increase of the dissociation probability by vibrational excitation than by translation per unit of energy is consistent with a late barrier along the O-D stretch reaction coordinate.
doi_str_mv 10.1126/science.1251277
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source JSTOR Archive Collection A-Z Listing; American Association for the Advancement of Science
subjects Biophysics
Chemical synthesis
Chemisorption
Chemistry
Coordinate systems
Energy
Methane
Molecular beams
Molecular chemistry
Molecular excitation
Molecules
Nozzles
Reactants
Reactivity
Vibrational states
Water
title Vibrationally Promoted Dissociation of Water on Ni(111)
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