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  Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil

Kaichev, V. V., Teschner, D., Saraev, A. A., Kosolobov, S. S., Gladky, A. Y., Prosvirin, I. P., et al. (2016). Evolution of self-sustained kinetic oscillations in the catalytic oxidation of propane over a nickel foil. Journal of Catalysis, 324, 23-33. doi:10.1016/j.jcat.2015.11.009.

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Kaichev, V. V.1, 2, Author
Teschner, Detre3, Author           
Saraev, A. A.1, 2, Author
Kosolobov, S. S.2, 4, Author
Gladky, A. Yu.1, Author
Prosvirin, I. P.1, Author
Rudina, N. A.1, Author
Ayupov, A. B.1, Author
Blume, Raoul3, 5, Author           
Hävecker, Michael3, 5, Author           
Knop-Gericke, Axel3, Author           
Schlögl, Robert3, Author           
Latyshev, A. V.4, Author
Bukhtiyarov, V. I.1, 2, Author
Affiliations:
1Boreskov Institute of Catalysis , Lavrentiev Ave. 5, 630090 Novosibirsk, Russia, ou_persistent22              
2Novosibirsk State University, Pirogov Str. 2, 630090 Novosibirsk, Russia, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Rzhanov Institute of Semiconductor Physics, Lavrentiev Ave. 13, 630090 Novosibirsk, Russia, ou_persistent22              
5Abt. Solarenergieforschung, Helmhotz-Zentrum Berlin, ou_persistent22              

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 Abstract: The evolution of self-sustained reaction-rate oscillations in the catalytic oxidation of propane over a nickel foil has been studied in situ using X-ray photoelectron spectroscopy coupled with online mass spectrometry and gas chromatography. Changes in the effective surface area and in the catalyst morphology under reaction conditions have been examined by scanning electron microscopy and a krypton adsorption technique. It is shown that the regular kinetic oscillations arise under oxygen-lean conditions. CO, CO2, H2, H2O, and propylene are detected as products. The conversion of propane oscillates in a range from 1% to 23%. During the half-periods with high activity, the main reaction pathway is the partial oxi- dation of propane: selectivity toward CO achieves 98%. In contrast, during the half-periods with low activity, the reaction proceeds through three competitive pathways: the partial oxidation of propane, the total oxidation of propane, and the dehydrogenation of propane to propylene. The driving force for the self-sustained kinetic oscillations is the periodic reoxidation of nickel. According to the Ni2p and O1s core-level spectra measured in situ, the high-active catalyst surface is represented by metallic nickel, whereas during the inactive half-periods the catalyst surface is covered with a thick layer of NiO. The intensity of O1s spectra follows the oscillations of O2 in the gas phase during the oxidation of propane. It is found that during the induction period before the regular oscillations appear, a rough and porous structure develops because of strong reconstruction of the catalyst surface. The thickness of the recon- structed layer is approximately 10–20 μm. This process is accompanied with at least an 80-fold increase in the effective surface area compared with a clean, non-treated nickel foil, which undoubtedly leads to a drastic increase in the number of active sites. We believe that it is the main reason for the induction period always being observed before the appearance of self-sustained oscillations in the catalytic oxidation of light hydrocarbons over catalysts with a low specific surface area (single crystals, foils, or wires). Moreover, without such reconstruction, the oscillations cannot arise due to low activity of such catalysts.

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 Dates: 2015-10-302015-07-232015-11-182015-12-172016-02
 Publication Status: Issued
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.jcat.2015.11.009
 Degree: -

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Title: Journal of Catalysis
Source Genre: Journal
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Publ. Info: Amsterdam : Elsevier
Pages: 11 Volume / Issue: 324 Sequence Number: - Start / End Page: 23 - 33 Identifier: ISSN: 0021-9517
CoNE: https://pure.mpg.de/cone/journals/resource/954922645027