Journalartikel

On the Nature of the Active State of Supported Ruthenium Catalysts Used for the Oxidation of Carbon Monoxide:  Steady-State and Transient Kinetics Combined with in Situ Infrared Spectroscopy


AutorenlisteAssmann, J; Narkhede, V; Khodeir, L; Löffler, E; Hinrichsen, O; Birkner, A; Over, H; Muhler, M

Jahr der Veröffentlichung2004

Seiten14634-14642

ZeitschriftJournal of Physical Chemistry B (Soft Condensed Matter and Biophysical Chemistry)

Bandnummer108

Heftnummer38

ISSN1520-6106

DOI Linkhttps://doi.org/10.1021/jp0401675

VerlagAmerican Chemical Society


Abstract

The oxidation of CO over Ru/MgO and Ru/SiO2 catalysts was
used as a simple model reaction to derive turnover frequencies at
atmospheric pressure, which were observed to agree with kinetic data
obtained under high-vacuum conditions with supported ruthenium catalysts
and the RuO2(110) single-crystal surface. Thus, it was
possible to bridge both the pressure and the materials gap. However, a
partial deactivation was observed initially, which was identified as an
activated process, both under net reducing and net oxidizing conditions.
Temperature-programmed reduction (TPR) experiments were performed
subsequently in the same reactor, to monitor the degree of oxidation, as
a function of the reaction temperature and the CO/O2
reactant feed ratio. Using in situ diffuse reflectance infrared Fourier
transform spectroscopy (DRIFTS) measurements, the structural changes of
the ruthenium catalysts during the oxidation of CO were confirmed, under
relevant reaction conditions. Under net reducing conditions, only
domains of RuO2 seem to exist on the metallic ruthenium
particles, whereas, under net oxidizing conditions, the ruthenium
particles were fully oxidized to bulk RuO2 particles, which may expose less-active facets, such as the RuO2(100)−c(2 × 2) surface.




Autoren/Herausgeber




Zitierstile

Harvard-ZitierstilAssmann, J., Narkhede, V., Khodeir, L., Löffler, E., Hinrichsen, O., Birkner, A., et al. (2004) On the Nature of the Active State of Supported Ruthenium Catalysts Used for the Oxidation of Carbon Monoxide:  Steady-State and Transient Kinetics Combined with in Situ Infrared Spectroscopy, Journal of Physical Chemistry B (Soft Condensed Matter and Biophysical Chemistry), 108(38), pp. 14634-14642. https://doi.org/10.1021/jp0401675

APA-ZitierstilAssmann, J., Narkhede, V., Khodeir, L., Löffler, E., Hinrichsen, O., Birkner, A., Over, H., & Muhler, M. (2004). On the Nature of the Active State of Supported Ruthenium Catalysts Used for the Oxidation of Carbon Monoxide:  Steady-State and Transient Kinetics Combined with in Situ Infrared Spectroscopy. Journal of Physical Chemistry B (Soft Condensed Matter and Biophysical Chemistry). 108(38), 14634-14642. https://doi.org/10.1021/jp0401675


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