Abstract
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 650kJmol−1 O2 for fluorites and ∼500kJmol−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.
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