Sciact
  • EN
  • RU

In situ XPS Study of Self-Sustained Oscillations in Catalytic Oxidation of Propane over Nickel Full article

Journal Surface Science
ISSN: 0039-6028
Output data Year: 2013, Volume: 609, Pages: 113-118 Pages count : 6 DOI: 10.1016/j.susc.2012.11.012
Tags Heterogeneous catalysis, In situ ambient-pressure XPS, Nickel, Propane oxidation, Self-sustained oscillations
Authors Kaichev V.V. 1 , Gladky A.Yu. 1 , Prosvirin I.P. 1 , Saraev A.A. 1 , Hävecker M. 2 , Knop-Gericke A. 2 , Schlögl R. 2 , Bukhtiyarov V.I. 1
Affiliations
1 Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Science, 5 Acad. Lavrentieva Pr., Novosibirsk 630090, Russia
2 Department of Inorganic Chemistry, Fritz Haber Institute of the Max Plank Society, Faradayweg 4-6, D-14195 Berlin, Germany

Funding (2)

1 Federal Agency for Scientific Organizations 81
2 Russian Foundation for Basic Research 11-03-00498

Abstract: Self-sustained oscillations in the propane oxidation over a nickel foil were studied in situ with the use of ambient-pressure X-ray photoelectron spectroscopy (XPS) coupled with on-line mass-spectrometry and gas chromatography (GC). Regular oscillations of a relaxation type were observed at 0.5 mbar in the temperature range of 600–750 °C in oxygen-deficient conditions. CO, CO2, H2, H2O, and propylene were detected as products. CO selectivity in active half-periods achieved 98% decreasing to 40–60% in inactive half-periods. It has been found that the chemical state of the catalyst drastically changes together with the oscillations of the catalytic activity. According to the Ni2p and O1s core-level spectra measured in situ, the active catalyst surface is represented by metallic nickel, whereas it is covered with a layer of NiO with a thickness of at least 3 nm during the inactive half-periods. It means that the oscillations in the propane oxidation over nickel are originated from the reversible bulk oxidation of Ni to NiO. We suggest that the propane oxidation over the metallic Ni surface occurs via the Langmuir–Hinshelwood mechanism, whereas the Mars–van Krevelen mechanism prevails when the reaction proceeds over NiO. The switching between the metallic surface and the oxide shows a significant change in the catalytic activity. According to GC measurements the activity of metallic nickel is approximately 40-fold higher than that of NiO.
Cite: Kaichev V.V. , Gladky A.Y. , Prosvirin I.P. , Saraev A.A. , Hävecker M. , Knop-Gericke A. , Schlögl R. , Bukhtiyarov V.I.
In situ XPS Study of Self-Sustained Oscillations in Catalytic Oxidation of Propane over Nickel
Surface Science. 2013. V.609. P.113-118. DOI: 10.1016/j.susc.2012.11.012 WOS Scopus РИНЦ ANCAN OpenAlex
Files: Full text from publisher
Dates:
Submitted: Jun 8, 2012
Accepted: Nov 27, 2012
Published online: Dec 5, 2012
Published print: Mar 1, 2013
Identifiers:
Web of science: WOS:000315609200019
Scopus: 2-s2.0-84873057560
Elibrary: 20424617
Chemical Abstracts: 2013:119879
Chemical Abstracts (print): 158:227191
OpenAlex: W2008796388
Citing:
DB Citing
Web of science 89
Scopus 89
Elibrary 82
OpenAlex 94
Altmetrics: