Effect of Dissolved Carbon on Activation of Methane on Palladium: Experimental and Theoretical Study | Sciact - CRIS-система Института катализа

Effect of Dissolved Carbon on Activation of Methane on Palladium: Experimental and Theoretical Study Научная публикация

Журнал

Catalysis Letters
ISSN: 1011-372X , E-ISSN: 1572-879X

Вых. Данные

Год: 2025, Том: 155, Номер: 9, Номер статьи : 303, Страниц : 12 DOI: 10.1007/s10562-025-05140-3

Ключевые слова

Palladium · Palladium carbide · Methane · Oxidation · Catalytic activity

Авторы

Kaichev Vasily V. ¹ , Laletina Svetlana S. ^1,2 , Vinokurov Zakhar S. ³ , Shor Elena A. ² , Yudanov Ilya V. ^1,4

Организации

1	Boreskov Institute of Catalysis SB RAS, Novosibirsk 630090, Russia
2	Federal Research Center “Krasnoyarsk Science Center SB RAS”, Institute of Chemistry and Chemical Technology of the Siberian Branch of the Russian Academy of Sciences, Krasnoyarsk 660036, Russia
3	Synchrotron Radiation Facility SKIF, Boreskov Institute of Catalysis, Koltsovo 630559, Russia
4	Institute of Solid State Chemistry and Mechanochemistry SB RAS, Novosibirsk 630128, Russia

Информация о финансировании (2)

1	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	075-00500-21-00 (FWES-2021-0012) (121031500209-6)
2	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	FWUR-2024-0032

Using experimental and theoretical methods, we studied the dissolution of carbon in near-surface layers of palladium, the formation of palladium carbide and its reactivity toward oxygen. By studying self-sustained oscillations during the oxidation of methane over Pd foil by X-ray diffraction and mass spectrometry, we found that the formation of palladium carbide proceeds simultaneously with a sharp increase in catalytic activity. However, ab initio calculations indicated that the dissolution of carbon in near-surface layers of palladium leads to increasing activation barriers of methane decomposition steps. For example, for the hydrogen abstraction from CH adsorbed species, the activation barrier increases from 54 to 80 kJ/mol. Since the C–H bond breaking activity is the limiting factor in the hydrocarbon oxidation, such increase means that the formation of palladium carbide leads to a decrease in the catalytic activity. Therefore, the formation of palladium carbide is a result of high activity of metallic palladium in the methane decomposition; the carbon formed in this case can not only accumulate on the surface, but also dissolve in the near-surface layers of palladium; both processes reduce the activity of palladium.

Kaichev V.V. , Laletina S.S. , Vinokurov Z.S. , Shor E.A. , Yudanov I.V.
Effect of Dissolved Carbon on Activation of Methane on Palladium: Experimental and Theoretical Study
Catalysis Letters. 2025. V.155. N9. 303 :1-12. DOI: 10.1007/s10562-025-05140-3 WOS Scopus CAPlus

Поступила в редакцию:	30 мая 2025 г.
Принята к публикации:	28 июл. 2025 г.
Опубликована в печати:	14 авг. 2025 г.
Опубликована online:	14 авг. 2025 г.

Web of science:	WOS:001550850100001
Scopus:	2-s2.0-105013174418
Chemical Abstracts:	2025:2005803

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