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Self-Sustained Oscillations in Oxidation of Methane over Palladium: The Nature of “Low-Active” and “Highly Active” States Full article

Journal Catalysis Science and Technology
ISSN: 2044-4753 , E-ISSN: 2044-4761
Output data Year: 2021, Volume: 11, Number: 13, Pages: 4392-4397 Pages count : 6 DOI: 10.1039/d1cy00132a
Tags CATALYST TEMPERATURE OSCILLATIONS; IN-SITU; CARBON-MONOXIDE; COMBUSTION; DEPENDENCE; PLATINUM; BEHAVIOR; Pd(111); NICKEL; PHASE
Authors Kaichev Vasily V. 1 , Vinokurov Zakhar S. 1 , Saraev Andrey A. 1
Affiliations
1 Boreskov Institute of Catalysis, Novosibirsk, Russia

Funding (2)

1 Russian Foundation for Basic Research 19-03-00419
2 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0003

Abstract: The oxidation of methane was studied in a flow reactor at atmospheric pressure using palladium foil as a catalyst. It was shown that regular self-sustained reaction rate oscillations occur under oxygen-deficient conditions. CO, CO2, H2, and H2O were detected as products when the catalyst was in a highly active state. The signals of CO and H2 were small, indicating that the total oxidation is the main reaction. According to the operando X-ray diffraction and mass spectrometry study, the driving force for the oscillations is periodic oxidation and reduction of palladium. The highly active state is palladium in the metallic state, and the transition to the low-active state is accompanied by the growth of a PdO film on the palladium surface. The decomposition of PdO is accompanied by the formation of a Pd carbide layer. This is a result of accumulation of carbon on the highly active surface of metallic palladium and its subsequent dissolution in the bulk of palladium. The dissolution of carbon in the subsurface layers of palladium has no a significant effect on its catalytic activity. The oscillatory mechanism for the oxidation of methane over palladium is discussed.
Cite: Kaichev V.V. , Vinokurov Z.S. , Saraev A.A.
Self-Sustained Oscillations in Oxidation of Methane over Palladium: The Nature of “Low-Active” and “Highly Active” States
Catalysis Science and Technology. 2021. V.11. N13. P.4392-4397. DOI: 10.1039/d1cy00132a WOS Scopus РИНЦ AN OpenAlex
Dates:
Submitted: Jan 26, 2021
Accepted: Apr 30, 2021
Published online: May 4, 2021
Published print: Jul 7, 2021
Identifiers:
Web of science: WOS:000652863200001
Scopus: 2-s2.0-85109218085
Elibrary: 46878590
Chemical Abstracts: 2021:1019928
OpenAlex: W3158283650
Citing:
DB Citing
Web of science 10
Scopus 12
Elibrary 13
OpenAlex 13
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