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Self-Sustained Oscillations in Oxidation of Propane Over Nickel: Experimental Study and Mathematical Modelling Full article

Общее Language: Английский, Genre: Full article,
Status: Published, Source type: Original
Conference XI International Conference Mechanisms of Catalytic Reactions
07-11 Oct 2019 , Сочи
Journal Topics in Catalysis
ISSN: 1022-5528 , E-ISSN: 1572-9028
Output data Year: 2020, Volume: 63, Number: 1-2, Pages: 33-48 Pages count : 16 DOI: 10.1007/s11244-019-01219-5
Tags Heterogeneous catalysis; Mathematical modelling; Nickel; Propane oxidation; Quasi-steady-state approximations; Self-sustained oscillations
Authors Lashina E.A. 1,2 , Kaichev V.V. 1,2 , Saraev A.A. 1,2 , Chumakova N.A. 1,2 , Chumakov G.A. 2,3 , Bukhtiyarov V.I. 1,2
Affiliations
1 Boreskov Institute of Catalysis, Novosibirsk, Russia 630090
2 Novosibirsk State University, Novosibirsk, Russia 630090
3 Sobolev Institute of Mathematics, Novosibirsk, Russia 630090

Funding (3)

1 Federal Agency for Scientific Organizations 0303-2016-0001
2 Federal Agency for Scientific Organizations 0303-2016-0017
3 Президиум СО РАН I.1.5.3

Abstract: The regular reaction rate oscillations were observed by mass-spectrometry in the oxidation of propane over the Ni foil. CO, CO2, H2, and H2O were detected as products. The oscillations of products and reactants in the gas phase were accompanied by the oscillations of the catalyst temperature. It was shown by using isotopic labeling 18O2 that CO and CO2 formed simultaneously by the propane oxidation when the catalyst was in the highly active state. The non-isothermal model of a continuous stirred-tank reactor based on a microkinetic scheme including 50 reaction steps was developed. The model takes into account periodic oxidation and reduction of nickel and formation of main products. Using the method of quasi-steady-state approximations, it was shown that the observed self-sustained oscillations are associated with periodic changes in the coverage of the Ni surface by adsorbed oxygen and carbon as well as nickel oxide species. It was shown that the microkinetic scheme coupled with a continuous stirred-tank reactor model qualitatively describes the experimental data if the model also considers the periodic processes of oxidation and reduction of the Ni bulk. © 2020, Springer Science+Business Media, LLC, part of Springer Nature.
Cite: Lashina E.A. , Kaichev V.V. , Saraev A.A. , Chumakova N.A. , Chumakov G.A. , Bukhtiyarov V.I.
Self-Sustained Oscillations in Oxidation of Propane Over Nickel: Experimental Study and Mathematical Modelling
Topics in Catalysis. 2020. V.63. N1-2. P.33-48. DOI: 10.1007/s11244-019-01219-5 publication_identifier_short.wos_identifier_type publication_identifier_short.scopus_identifier_type publication_identifier_short.rinz_identifier_type
Dates:
Published online: Feb 3, 2020
Published print: Mar 1, 2020
Identifiers:
publication_identifier.wos_identifier_type WOS:000515805600003
publication_identifier.scopus_identifier_type 2-s2.0-85079146397
publication_identifier.rinz_identifier_type 43239498
publication_identifier.accession_number_identifier_type 2020:296620
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