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In Situ NAP-XPS and Mass Spectrometry Study of the Oxidation of Propylene over Palladium Full article

Общее Language: Английский, Genre: Full article,
Status: Published, Source type: Original
Journal The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455
Output data Year: 2018, Volume: 122, Number: 8, Pages: 4315-4323 Pages count : 9 DOI: 10.1021/acs.jpcc.7b11129
Tags RAY PHOTOELECTRON-SPECTROSCOPY; SUSTAINED KINETIC OSCILLATIONS; AMBIENT-PRESSURE XPS; CATALYTIC-OXIDATION; METHANE OXIDATION; ELECTRON-MICROSCOPY; ETHENE OXIDATION; PD(111); NICKEL; MBAR
Authors Kaichev Vasily V. 1,2 , Saraev Andrey A. 1,2 , Matveev Andrey V. 1,2 , Dubinin Yury V. 1 , Knop-Gericke Axel 3 , Bukhtiyarov Valerii I. 1,2
Affiliations
1 Boreskov Institute of Catalysis, Lavrentieva Ave. 5, 630090 Novosibirsk, Russia
2 Novosibirsk State University, Pirogova Str. 2, 630090 Novosibirsk, Russia
3 Department of Inorganic Chemistry, Fritz Haber Institute, Faradayweg 4-6, D-14195 Berlin, Germany

Funding (1)

1 Federal Agency for Scientific Organizations 0303-2016-0001

Abstract: The oxidation of propylene over a Pd(551) single crystal has been studied in the millibar pressure range using near-ambient pressure X-ray photoelectron spectroscopy and mass spectrometry. It has been shown that, irrespective of the O2/C3H6 molar ratio in the range 1–100, the total oxidation of propylene to CO2 and water and the partial oxidation of propylene to CO and H2 occur when the catalyst is heated above the light-off temperature; increasing the partial pressure of O2 leads to decreasing the catalytic activity. The selectivity toward CO2 is at least two times higher than the selectivity toward CO, indicating that the total oxidation is the main reaction route. The normal hysteresis with a light-off temperature higher than the extinction temperature is observed in the oxidation of propylene between 100 and 300 °C. According to NAP-XPS, the main reason for the hysteresis appearing is a competition between two surface processes: carbonization and oxidation of palladium. At low temperatures, the adsorption and following decomposition of propylene dominate, which results in accumulation of carbonaceous deposits blocking the palladium surface. Increasing the catalyst temperature leads to burning the carbonaceous deposits which initiates the following oxidation of propylene. The highest conversion of propylene is observed when both free surface sites and adsorbed oxygen atoms exist in a large amount on the catalyst surface. As the partial pressure of O2 increases, the catalyst surface gets covered by clusters of surface 2D palladium oxide, which is accompanied by a decrease in the catalytic activity. The mechanism of the oxidation of propylene over palladium is discussed.
Cite: Kaichev V.V. , Saraev A.A. , Matveev A.V. , Dubinin Y.V. , Knop-Gericke A. , Bukhtiyarov V.I.
In Situ NAP-XPS and Mass Spectrometry Study of the Oxidation of Propylene over Palladium
The Journal of Physical Chemistry C. 2018. V.122. N8. P.4315-4323. DOI: 10.1021/acs.jpcc.7b11129 publication_identifier_short.wos_identifier_type publication_identifier_short.scopus_identifier_type publication_identifier_short.rinz_identifier_type
Dates:
Submitted: Nov 10, 2017
Published online: Feb 21, 2018
Published print: Mar 1, 2018
Identifiers:
publication_identifier.wos_identifier_type WOS:000426802500024
publication_identifier.scopus_identifier_type 2-s2.0-85042792381
publication_identifier.rinz_identifier_type 35543300
publication_identifier.accession_number_identifier_type 2018:266967
publication_identifier.chemical_accession_number_identifier_type 169:156593
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