Mechanism of Ethanol Steam Reforming Over Pt/(Ni+Ru)-Promoted Oxides by FTIRS In Situ
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Конференция |
EuropaCat-XII: 12th European Congress on Catalysis “Catalysis: Balancing the use of fossil and renewable resources”
30 авг. - 4 сент. 2015
,
Казань
|
| Журнал |
Topics in Catalysis
ISSN: 1022-5528
, E-ISSN: 1572-9028
|
| Вых. Данные |
Год: 2016,
Том: 59,
Номер: 15,
Страницы: 1332-1342
Страниц
: 11
DOI:
10.1007/s11244-016-0659-y
|
| Ключевые слова |
DRIFT in situ, Ethanol, Mechanism, Reactivity, Steam reforming, Surface species |
| Авторы |
Sadykov Vladislav A.
1,2
,
Chub Olga V.
1
,
Chesalov Yurii A.
1
,
Mezentseva Natalia V.
1,2
,
Pavlova Svetlana N.
1
,
Arapova Marina V.
1,3
,
Rogov Vladimir A.
1,2
,
Simonov Mikhail N.
1,2
,
Roger Anne-Cecile
3
,
Parkhomenko Ksenia V.
3
,
van Veen Andre C.
4
|
| Организации |
| 1 |
Boreskov Institute of Catalysis, Prospekt Lavrentieva, 5, 630090 Novosibirsk, Russia
|
| 2 |
Novosibirsk State University, Pirogova st., 2, 630090 Novosibirsk, Russia
|
| 3 |
University of Strasbourg, Strasbourg, France
|
| 4 |
University of Warwick, Coventry, UK
|
|
Информация о финансировании (4)
|
1
|
Министерство образования и науки Российской Федерации
|
|
|
2
|
European Commission
|
604296 FP7-NMP-2013-LARGE-7 BIOGO
|
|
3
|
Российский фонд фундаментальных исследований
|
15-53-16020
|
|
4
|
Российский фонд фундаментальных исследований
|
12-03-93115
|
Mechanism of ethanol steam reforming into syngas over Pt/Pr0.15Sm0.15Ce0.35Zr0.35O2 and 10 wt% LaNi0.9Ru0.1O3/Mg-Al2O3 catalysts was studied by in situ FTIRS and pulse titration experiments. Surface species (ethoxy, adsorbed ethanol, acetaldehyde, acetate, etc.) were identified and their thermal stability, routers of transformation and reactivity were characterized. Acetate species were shown to be spectators for both types of catalysts. Transformation of ethoxy species by dehydrogenation is a fast step, while the rate-determining stage is the C–C bond rupture in thus formed acetaldehyde on metal sites. For Pt/Pr0.15Sm0.15Ce0.35Zr0.35O2 catalyst with a high mobility and reactivity of the surface/lattice oxygen of support, efficient oxidative transformation of acetaldehyde at the metal-support interface provides a high yield of syngas at short contact times in the intermediate temperature range with a minor amount of CH4 by-product. Transformation of ethoxy species on the acid sites of alumina-supported catalyst produces C2H4 and (C2H5)2O via dehydration route dominating at temperatures below 400 °C. In addition, for alumina-supported catalyst acetone is produced via aldol formation in the temperature range 400–500 °C due to combined action of metal and support sites. For this catalyst syngas yield is improved at high temperatures when steam reforming of these byproducts efficiently proceeds accompanied by cracking reactions producing also methane as by-product.