In situ XPS Study of Self-Sustained Oscillations in Catalytic Oxidation of Propane over Nickel | Sciact - CRIS-система Института катализа

In situ XPS Study of Self-Sustained Oscillations in Catalytic Oxidation of Propane over Nickel Научная публикация

Журнал

Surface Science
ISSN: 0039-6028

Вых. Данные

Год: 2013, Том: 609, Страницы: 113-118 Страниц : 6 DOI: 10.1016/j.susc.2012.11.012

Ключевые слова

Heterogeneous catalysis, In situ ambient-pressure XPS, Nickel, Propane oxidation, Self-sustained oscillations

Авторы

Kaichev V.V. ¹ , Gladky A.Yu. ¹ , Prosvirin I.P. ¹ , Saraev A.A. ¹ , Hävecker M. ² , Knop-Gericke A. ² , Schlögl R. ² , Bukhtiyarov V.I. ¹

Организации

1	Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Science, 5 Acad. Lavrentieva Pr., Novosibirsk 630090, Russia
2	Department of Inorganic Chemistry, Fritz Haber Institute of the Max Plank Society, Faradayweg 4-6, D-14195 Berlin, Germany

Информация о финансировании (2)

1	Федеральное агентство научных организаций России	81
2	Российский фонд фундаментальных исследований	11-03-00498

Self-sustained oscillations in the propane oxidation over a nickel foil were studied in situ with the use of ambient-pressure X-ray photoelectron spectroscopy (XPS) coupled with on-line mass-spectrometry and gas chromatography (GC). Regular oscillations of a relaxation type were observed at 0.5 mbar in the temperature range of 600–750 °C in oxygen-deficient conditions. CO, CO2, H2, H2O, and propylene were detected as products. CO selectivity in active half-periods achieved 98% decreasing to 40–60% in inactive half-periods. It has been found that the chemical state of the catalyst drastically changes together with the oscillations of the catalytic activity. According to the Ni2p and O1s core-level spectra measured in situ, the active catalyst surface is represented by metallic nickel, whereas it is covered with a layer of NiO with a thickness of at least 3 nm during the inactive half-periods. It means that the oscillations in the propane oxidation over nickel are originated from the reversible bulk oxidation of Ni to NiO. We suggest that the propane oxidation over the metallic Ni surface occurs via the Langmuir–Hinshelwood mechanism, whereas the Mars–van Krevelen mechanism prevails when the reaction proceeds over NiO. The switching between the metallic surface and the oxide shows a significant change in the catalytic activity. According to GC measurements the activity of metallic nickel is approximately 40-fold higher than that of NiO.

Kaichev V.V. , Gladky A.Y. , Prosvirin I.P. , Saraev A.A. , Hävecker M. , Knop-Gericke A. , Schlögl R. , Bukhtiyarov V.I.
In situ XPS Study of Self-Sustained Oscillations in Catalytic Oxidation of Propane over Nickel

Surface Science. 2013. V.609. P.113-118. DOI: 10.1016/j.susc.2012.11.012 WOS Scopus РИНЦ CAPlusCA OpenAlex

Полный текст от издателя

Поступила в редакцию:	8 июн. 2012 г.
Принята к публикации:	27 нояб. 2012 г.
Опубликована online:	5 дек. 2012 г.
Опубликована в печати:	1 мар. 2013 г.

Web of science:	WOS:000315609200019
Scopus:	2-s2.0-84873057560
РИНЦ:	20424617
Chemical Abstracts:	2013:119879
Chemical Abstracts (print):	158:227191
OpenAlex:	W2008796388

БД	Цитирований
Web of science	89
Scopus	89
РИНЦ	82
OpenAlex	94