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Carbon dioxide activation and alkali compound formation. I: Vibrational characterization of oxalate intermediates
Luleå tekniska universitet, Institutionen för teknikvetenskap och matematik, Materialvetenskap.
Jefferson Lab.
SCI-MED, New York.
2003 (engelsk)Inngår i: Surface Science, ISSN 0039-6028, E-ISSN 1879-2758, Vol. 531, nr 3, s. 244-264Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

The activation of CO2 in thin potassium layers adsorbed on Cu(1 1 1) has been studied with time-evolved Fourier transform-infrared reflection absorption spectroscopy. The growth of thin layers by reactive evaporation of potassium in a CO2 atmosphere permits control of the K:CO2 stoichiometry, which strongly affects the selectivity in the formation of intermediates and the decomposition pathways of the layer. Layers grown in a CO2 rich atmosphere exhibit the preferential growth of stoichiometric potassium oxalate K2C2O4 (D2h). The molecular identity of oxalate with D2h symmetry is confirmed by vibrational spectra utilizing isotopic substitution methods (13CO2 and C18O2) and by the use of isotopic mixtures of CO2/C18O2 and CO2/13CO2. A comparison of the isotope data with theoretical calculations gives an estimated OCO bond angle in oxalate of 132°. Far-IR spectra obtained with synchrotron radiation indicate the equivalent interaction of all oxygen atoms with the potassium. A comparison of the vibrational data with theoretical ab initio calculations confirms the structural model of an oxalate species that is bulk coordinated with no strong directional bonding and all oxygen atoms equally interacting with potassium. At medium and low CO2:K ratios, very complex vibrational spectra are observed, indicating the formation of an oxalate surface species with C2v symmetry in addition to D2h- oxalate, CO2- and CO22- species.

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2003. Vol. 531, nr 3, s. 244-264
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URN: urn:nbn:se:ltu:diva-10383DOI: 10.1016/S0039-6028(03)00511-9ISI: 000183254900010Scopus ID: 2-s2.0-0038750607Lokal ID: 92fb6c80-f1bf-11db-bb1b-000ea68e967bOAI: oai:DiVA.org:ltu-10383DiVA, id: diva2:983325
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Validerad; 2003; 20070423 (ysko)Tilgjengelig fra: 2016-09-29 Laget: 2016-09-29 Sist oppdatert: 2018-07-10bibliografisk kontrollert

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