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Infrared-induced reactivity of N2O on small gas-phase rhodium clusters
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Hamilton, Suzanne M., Hopkins, W. Scott, Harding, Dan J., Walsh, Tiffany R., Haertelt, Marko, Kerpal, Christian, Gruene, Philipp, Meijer, Gerard, Fielicke, André and Mackenzie, Stuart R. (2011) Infrared-induced reactivity of N2O on small gas-phase rhodium clusters. Journal of Physical Chemistry A, Volume 115 (Number 12). pp. 2489-2497. doi:10.1021/jp201171p ISSN 1089-5639.
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Official URL: http://dx.doi.org/10.1021/jp201171p
Abstract
Far- and mid-infrared multiple photon dissociation spectroscopy has been employed to study both the structure and surface reactivity of isolated cationic rhodium clusters with surface-adsorbed nitrous oxide, RhnN2O+ (n = 4−8). Comparison of experimental spectra recorded using the argon atom tagging method with those calculated using density functional theory (DFT) reveals that the nitrous oxide is molecularly bound on the rhodium cluster via the terminal N-atom. Binding is thought to occur exclusively on atop sites with the rhodium clusters adopting close-packed structures. In related, but conceptually different experiments, infrared pumping of the vibrational modes corresponding with the normal modes of the adsorbed N2O has been observed to result in the decomposition of the N2O moiety and the production of oxide clusters. This cluster surface chemistry is observed for all cluster sizes studied except for n = 5. Plausible N2O decomposition mechanisms are given based on DFT calculations using exchange-correlation functionals. Similar experiments pumping the Rh−O stretch in RhnON2O+ complexes, on which the same chemistry is observed, confirm the thermal nature of this reaction.
Item Type: | Journal Article | ||||
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Subjects: | Q Science > QD Chemistry | ||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||
Library of Congress Subject Headings (LCSH): | Rhodium, Metal clusters, Nitrous oxide -- Reactivity, Infrared spectroscopy | ||||
Journal or Publication Title: | Journal of Physical Chemistry A | ||||
Publisher: | American Chemical Society | ||||
ISSN: | 1089-5639 | ||||
Official Date: | 31 March 2011 | ||||
Dates: |
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Volume: | Volume 115 | ||||
Number: | Number 12 | ||||
Page Range: | pp. 2489-2497 | ||||
DOI: | 10.1021/jp201171p | ||||
Status: | Peer Reviewed | ||||
Publication Status: | Published | ||||
Access rights to Published version: | Restricted or Subscription Access | ||||
Funder: | European Union (EU), Engineering and Physical Sciences Research Council (EPSRC), Deutsche Forschungsgemeinschaft (DFG), University College, London. Ramsay Memorial Fellowships Trust, University of Warwick. Institute of Advanced Study, Alexander von Humboldt-Stiftung | ||||
Grant number: | EP/C012070 (EPSRC), EP/C01202X (EPSRC) |
Data sourced from Thomson Reuters' Web of Knowledge
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