Mechanism of CH4 Dry Reforming by Pulse Microcalorimetry: Metal Nanoparticles on Perovskite/Fluorite Supports with High Oxygen Mobility | Sciact - CRIS-system of Boreskov Institute of Catalysis

Mechanism of CH4 Dry Reforming by Pulse Microcalorimetry: Metal Nanoparticles on Perovskite/Fluorite Supports with High Oxygen Mobility Full article

Journal

Thermochimica Acta
ISSN: 0040-6031 , E-ISSN: 1872-762X

Output data

Year: 2013, Volume: 567, Pages: 27- 34 Pages count : 8 DOI: 10.1016/j.tca.2013.01.034

Tags

Bonding strength and reactivity of oxygen species, CH4 dry reforming, Metal clusters, Perovskite and fluorite oxide supports, Pulse microcalorimetry, Redox mechanism

Authors

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

Affiliations

1	Boreskov Institute of Catalysis, Novosibirsk, Russia
2	Novosibirsk State University, Novosibirsk, Russia
3	Institut de Recherches sur la catalyse et l’environnement de Lyon, France

Funding (4)

1	Russian Foundation for Basic Research	09-03-93112
2	French Embassy in Moscow
3	The Ministry of Education and Science of the Russian Federation
4	European Commission	228953 FP7-NMP-2008-LARGE-2 OCMOL

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.

Sadykov V. , Rogov V. , Ermakova E. , Arendarsky D. , Mezentseva N. , Alikina G. , Sazonova N. , Bobin A. , Pavlova S. , Schuurman Y. , Mirodatos C.
Mechanism of CH4 Dry Reforming by Pulse Microcalorimetry: Metal Nanoparticles on Perovskite/Fluorite Supports with High Oxygen Mobility
Thermochimica Acta. 2013. V.567. P.27- 34. DOI: 10.1016/j.tca.2013.01.034 WOS Scopus РИНЦ ANCAN OpenAlex

Submitted:	Oct 15, 2012
Accepted:	Jan 30, 2013
Published online:	Feb 16, 2013
Published print:	Sep 10, 2013

Web of science:	WOS:000323408100005
Scopus:	2-s2.0-84884531205
Elibrary:	20457146
Chemical Abstracts:	2013:341407
Chemical Abstracts (print):	160:76351
OpenAlex:	W2048247337

DB	Citing
Web of science	29
Scopus	30
Elibrary	28
OpenAlex	31