Abstract
The effect of Al2O3, TiO2, ZrO2 and Yttria-Stabilized Zirconia (YSZ) supports on the activity of the dry reforming of CH4 towards syngas production was investigated for Rh and Ru catalysts. Ruthenium-based catalysts were found to generally be more active than Rh leading H2/CO ratios close to unity above 700 °C. Methane conversion turnover frequency (TOF) over Rh catalysts becomes optimum for Rh/YSZ followed by Rh/TiO2 and Rh/ZrO2, and finally Rh/Al2O3, which exhibited the lowest activity. The performance order is different for Ru catalysts, with TOF being increased in the order Ru/Al2O3<Ru/TiO2<Ru/YSZ < Ru/ZrO2. Time-on-stream (TOS) stability tests showed that Rh/ZrO2 is stable for 30 h, whereas Ru/ZrO2 exhibits a slight decrease of both reactants’ conversions. DRIFTS studies indicated that the reaction proceeds via a bifunctional mechanism involving both the metal and the support in the reaction pathway. The population and adsorption sites of produced carbonyls are strongly influenced by the metal-support combination determining the catalytic activity.
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