Oscillations during partial oxidation of methane to synthesis gas over Ru/Al_2O_3 catalyst

Oscillations in temperatures of catalyst bed as well as concentrations of gas phase species at the exit of reactor were observed during the partial oxidation of methane to synthesis gas over Ru/Al_2O_3 in the temperature range of 600 to 850 ℃. XRD,H_2-TPR and in situ Raman techniques was used to characterize the catalyst. Two types of ruthenium species,i.e. the rutbenium species weakly interacted with Al_2O_3 and that strongly interacted with the support,were identified by H2-TPR experiment. These species are responsible for two types of oscillation profiles observed during the reaction. The oscillations were the result of these ruthenium species switching cyclically between the oxidized state and the reduced state under the reaction condition. These cyclic transformations,in turn,were the result of temperature variations caused by the varying levels of the strongly exothermic CH_4 combustion and the highly endothermic CH4 reforming (with H_2O and CO_2) reactions (or the less exothermic direct partial oxidation of methane to CO and H_2),which were favored by the oxidized and the metallic sites,respectively. The major pathway of synthesis gas formation over the catalyst was via the combustion-reforming mechanism.