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Modeling of Transient Studies on the Reaction Kinetics over Catalysts with Lattice Oxygen Mobility: Dry Reforming of CH4 over a Pt/PrCeZrO Catalyst Full article

Journal Chemical Engineering Journal
ISSN: 1385-8947 , E-ISSN: 1873-3212
Output data Year: 2018, Volume: 343, Pages: 530-543 Pages count : 14 DOI: 10.1016/j.cej.2018.03.037
Tags Transient studies; Kinetic modeling; Lattice oxygen mobility; Active oxide support; CH4 dry reforming; Pt promoted catalyst
Authors Mirodatos C. 1 , van Veen A.C. 2 , Pokrovskaya S.A. 3,4 , Chumakova N.A. 3,4 , Sazonova N.N. 3 , Sadykov V.A. 3,4
Affiliations
1 Institut de Recherches sur la Catalyse et l’Environnement de Lyon, Lyon, France
2 University of Warwick, School of Engineering, Coventry CV4 7AL, United Kingdom
3 Boreskov Institute of Catalysis SB RAS, 630090 Novosibirsk, Russia
4 Novosibirsk State University, 630090 Novosibirsk, Russia

Funding (6)

1 European Commission 228953 FP7-NMP-2008-LARGE-2 OCMOL
2 European Commission 604296 FP7-NMP-2013-LARGE-7 BIOGO
3 Federal Agency for Scientific Organizations 0303-2016-0013
4 Federal Agency for Scientific Organizations 0303-2016-0017
5 Siberian Branch of the Russian Academy of Sciences 80
6 The Ministry of Education and Science of the Russian Federation

Abstract: Dynamics of red-ox reactions occurring over catalysts with active oxide support is described by mathematical modeling. Numerical analysis is applied to transients from an initially oxidized state of a Pt/PrCeZrO catalyst to a partially reduced steady state present during CH4 dry reforming. Oxygen transport to the surface from adjacent regions in the catalyst lattice is considered to quantify the impact on the transient behavior in the model red-ox reaction over the catalyst with a high lattice oxygen mobility. Chemical transformations and coverages at the catalyst surface are largely affected by the internal transport of oxygen species, while the overall character and shape of transient curves remain defined by the specificity of the reaction kinetic scheme. Detailed analysis of CH4 dry reforming over a Pt/PrCeZrO catalyst at contact times of 4.7, 8, and 15 ms allowed to (1) clarify the factors that control dynamic system behavior and catalytic properties, (2) discriminate kinetic schemes, (3) confirm a high efficiency of cationic Pt species in CH4 dissociation, and (4) underpin that CO2 transformation may occur via carbonate intermediates located on oxidized Ptn+−-Pr4+-O surface sites. Direct estimation of bulk oxygen diffusion rate as well as kinetic parameters was carried out. Findings are consistent with the characteristics of the catalyst surface state and oxygen mobility in the surface/bulk layers.
Cite: Mirodatos C. , van Veen A.C. , Pokrovskaya S.A. , Chumakova N.A. , Sazonova N.N. , Sadykov V.A.
Modeling of Transient Studies on the Reaction Kinetics over Catalysts with Lattice Oxygen Mobility: Dry Reforming of CH4 over a Pt/PrCeZrO Catalyst
Chemical Engineering Journal. 2018. V.343. P.530-543. DOI: 10.1016/j.cej.2018.03.037 WOS Scopus РИНЦ AN OpenAlex
Files: Full text from publisher
Dates:
Submitted: Dec 21, 2017
Accepted: Mar 7, 2018
Published online: Mar 9, 2018
Published print: Jul 1, 2018
Identifiers:
Web of science: WOS:000430269200056
Scopus: 2-s2.0-85043538947
Elibrary: 35508320
Chemical Abstracts: 2018:469093
OpenAlex: W2794410976
Citing:
DB Citing
Web of science 22
Scopus 22
Elibrary 21
OpenAlex 22
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