Partial Oxidation of Methane on Pt-Supported Lanthanide Doped Ceria-Zirconia Oxides: Effect of the Surface/Lattice Oxygen Mobility on Catalytic Performance
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Catalysis Today
ISSN: 0920-5861
, E-ISSN: 1873-4308
|
| Вых. Данные |
Год: 2011,
Том: 169,
Номер: 1,
Страницы: 125-137
Страниц
: 13
DOI:
10.1016/j.cattod.2010.10.098
|
| Ключевые слова |
Fluorite-like oxides, Mechanism, Oxygen isotope exchange, Oxygen mobility and reactivity, Pt, Selective oxidation of CH4, Syngas, Transient studies |
| Авторы |
Sadykov Vladislav A.
1,2
,
Sazonova Nathalia N.
1
,
Bobin Aleksei S.
1,4
,
Muzykantov Vitalii S.
1
,
Gubanova Elena L.
1,3
,
Alikina Galina M.
1
,
Lukashevich Anton I.
1
,
Rogov Vladimir A.
1
,
Ermakova Eugenia N.
2
,
Sadovskaya Ekaterina M.
1
,
Mezentseva Nathalia V.
1
,
Zevak Ekaterina G.
2
,
Veniaminov Sergei A.
1
,
Muhler Martin
3
,
Mirodatos Claude
4
,
Schuurman Yves
4
,
van Veen Andre C.
3,4
|
| Организации |
| 1 |
Boreskov Institute of Catalysis SB RAS, Pr. Lavrentieva 5, Novosibirsk 630090, Russia
|
| 2 |
Novosibirsk State University, Pirogova, 2, Novosibirsk 630090, Russia
|
| 3 |
Lehrstuhl für Technische Chemie, Ruhr-Universität Bochum, Universitätsstraße 150, 44780 Bochum, Germany
|
| 4 |
Institut de Recherches sur la catalyse et l’environnement de Lyon (IRCELYON), UMR 5256 (CNRS/Université Claude Bernard Lyon1),
Université de Lyon – Université Claude Bernard Lyon1, 2 Avenue Albert Einstein, Villeurbanne Cedex 69626, France
|
|
Информация о финансировании (5)
|
1
|
European Commission
|
228953 FP7-NMP-2008-LARGE-2 OCMOL
|
|
2
|
Российский фонд фундаментальных исследований
|
09-03-93112
|
|
3
|
Министерство образования и науки Российской Федерации
|
|
|
4
|
German Research Foundation
|
SFB 558
|
|
5
|
Посольство Франции в России
|
|
Partial oxidation of methane into syngas at short contact times (5–15 ms) was studied in both steady-state and transient modes at temperatures up to 850 °C in realistic feeds (CH4 content up to 20%, CH4/O2 = 2) with a minimum impact of mass and heat transfer for structured catalysts carrying Pt/Ln0.3Ce0.35Zr0.35O2−y (Ln = La, Pr, Gd) as thin layers on walls of corundum channel substrates. Oxygen mobility and reactivity of the active phase were characterized by oxygen isotope heteroexchange, temperature-programmed O2 desorption and CH4 reduction, isothermal pulse reduction by methane with wide variation of CH4 concentrations and TAP pulse studies. Experimental data point towards a selective oxidation of methane into syngas via a direct route with oxygen-assisted methane activation. This mechanistic feature is related to the strong Pt-support interaction stabilizing highly dispersed oxidic Pt species less active in CH4 and syngas combustion than metallic Pt clusters. Support activates O2 molecules and supplies active oxygen species to Pt sites. A high rate of oxygen diffusion on the surface and in the bulk of the support and Pt-support oxygen spillover stabilizes Pt in a well dispersed partially oxidized state while preventing coking at high concentrations of CH4 in the feed.