Mechanism of CH4 Dry Reforming by Pulse Microcalorimetry: Metal Nanoparticles on Perovskite/Fluorite Supports with High Oxygen Mobility
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Thermochimica Acta
ISSN: 0040-6031
, E-ISSN: 1872-762X
|
| Вых. Данные |
Год: 2013,
Том: 567,
Страницы: 27- 34
Страниц
: 8
DOI:
10.1016/j.tca.2013.01.034
|
| Ключевые слова |
Bonding strength and reactivity of oxygen species, CH4 dry reforming, Metal clusters, Perovskite and fluorite oxide supports, Pulse microcalorimetry, Redox mechanism |
| Авторы |
Sadykov Vladislav
1,2
,
Rogov Vladimir
1,2
,
Ermakova Eugenia
2
,
Arendarsky Dmitry
1
,
Mezentseva Natalia
1,2
,
Alikina Galina
1
,
Sazonova Natalia
1
,
Bobin Aleksey
1
,
Pavlova Svetlana
1
,
Schuurman Yves
3
,
Mirodatos Claude
3
|
| Организации |
| 1 |
Институт катализа им. Г.К. Борескова СО РАН
|
| 2 |
Новосибирский национальный исследовательский государственный университет
|
| 3 |
Institute of Researches on Catalysis and Environment in Lyon
|
|
Информация о финансировании (4)
|
1
|
European Commission
|
228953 FP7-NMP-2008-LARGE-2 OCMOL
|
|
2
|
Российский фонд фундаментальных исследований
|
09-03-93112
|
|
3
|
Посольство Франции в России
|
|
|
4
|
Министерство образования и науки Российской Федерации
|
|
The mechanism of CH4 dry reforming on Pt, Ru, Ni, Ni + Ru-supported perovskite (PrFeOx, LaPrMnCrOx) or fluorite (LnCeZrOx) oxides was studied using a Setaram Sensys DSC TG calorimeter and a pulse kinetic installation. For catalysts in the steady-state, CH4 and CO2 transformation in separate pulses proceeds with the rate and products selectivity equal to that in mixed CO2 + CH4 pulses. Heat effects of separate stages correspond to CH4 oxidation into syngas by strongly bound bridging oxygen forms of support (heat of adsorption up to 650 kJ mol−1 O2 for fluorites and ∼500 kJ mol−1 O2 for perovskites) and their replenishment by CO2 dissociation, respectively. These features demonstrate a step-wise red-ox (Mars-van-Crevelen) mechanism of CH4 dry reforming. Fast oxygen transfer from the sites of oxide support to the metal/oxide interface provides required conjugation of stages.