期刊
THERMOCHIMICA ACTA
卷 567, 期 -, 页码 27-34出版社
ELSEVIER
DOI: 10.1016/j.tca.2013.01.034
关键词
CH4 dry reforming; Metal clusters; Perovskite and fluorite oxide supports; Redox mechanism; Pulse microcalorimetry; Bonding strength and reactivity of oxygen species
资金
- OCMOL FP7 Project
- RFBR-CNRS [09-03-93112]
- Russian Federal Innovation Agency
- Embassy of France in Moscow
The mechanism of CH4 dry reforming on Pt, Ru, Ni, Ni + Ru-supported perovskite (PrFeOx, LaPrMnCrOx) or fluorite (LnCeZrO(x)) 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) O-2 for fluorites and similar to 500 kJ mol(-1) O-2 for perovskites) and their replenishment by CO2 dissociation, respectively. These features demonstrate a step-wise red-ox (Marsvan-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. (C) 2013 Elsevier B.V. All rights reserved.
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