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Self‐Sustained Oscillations within the Temperature Hysteresis in CO Oxidation over Pd: Mathematical Model of a Cascade of Continuous Stirred‐Tank Reactors Full article

Journal International Journal of Chemical Kinetics
ISSN: 0538-8066 , E-ISSN: 1097-4601
Output data Year: 2019, Volume: 51, Number: 12, Pages: 918-930 Pages count : 13 DOI: 10.1002/kin.21320
Tags a cascade of continuous stirred‐tank reactors, CO oxidation reaction, inverse temperature hysteresis, palladium bulk oxide, self‐sustained oscillations,transformations of the palladium structure
Authors Lashina E.A. 1,3 , Slavinskaya E.M. 1,3 , Chumakova N.A. 1,3 , Chumakov G.A. 2,3 , Boronin A.I. 1,3
Affiliations
1 Boreskov Institute of Catalysis, Novosibirsk, Russian Federation
2 Sobolev Institute of Mathematics, Novosibirsk, Russian Federation
3 Novosibirsk State University, Novosibirsk, Russian Federation

Abstract: The results of temperature-programmed reaction experimental studies and mathematical modeling of self-sustained oscillations within an inverse temperature hysteresis in CO oxidation over Pd catalyst are presented. The experimental data demonstrate the influence of the reaction medium on the catalyst activity under reaction conditions. Under oxygen excess in the feeding gas mixture and high temperature, the defects appeared on the initially flat surface of metallic palladium due to deep oxidation of palladium (three-dimensional PdO nanoparticles were observed). The palladium oxide reduced under cooling of the catalytic system, and the catalyst surface became flat again. To take into account these variations of the palladium surface structure, we consider the piecewise-constant dependence of the rate constant of some reaction step on the concentrations of oxygen species, namely, the dissolved oxygen or oxide in the palladium bulk. The proposed model of the process in the cascade of continuous stirred-tank reactors that account for these dependences qualitatively describes the inverse temperature hysteresis as well as the oscillatory dynamics within the hysteresis loop which were obtained experimentally.
Cite: Lashina E.A. , Slavinskaya E.M. , Chumakova N.A. , Chumakov G.A. , Boronin A.I.
Self‐Sustained Oscillations within the Temperature Hysteresis in CO Oxidation over Pd: Mathematical Model of a Cascade of Continuous Stirred‐Tank Reactors
International Journal of Chemical Kinetics. 2019. V.51. N12. P.918-930. DOI: 10.1002/kin.21320 WOS Scopus OpenAlex
Dates:
Submitted: Apr 1, 2019
Accepted: Sep 3, 2019
Published online: Sep 19, 2019
Published print: Dec 10, 2019
Identifiers:
Web of science: WOS:000487433600001
Scopus: 2-s2.0-85073435209
OpenAlex: W2974690670
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