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Pd/Al2O3 catalysts oscillate between ignition and extinction of the catalytic partial oxidation of methane when they are exposed to a 2:1 reaction mixture of methane and oxygen. The oscillations of the catalytic performance and the structure of Pd/Al2O3 catalysts in a fixed-bed reactor were investigated using spatially and time-resolved in situ quick scanning X-ray absorption spectroscopy with online mass spectrometry. The dynamic methane conversion oscillated between an inactive state, where only combustion occurred, and an active state, after ignition, where partial oxidation of methane as a combination of total oxidation and reforming in the catalytic capillary reactor was observed. This change in catalytic performance was directly linked to changes in the oxidation state of the Pd/Al2O3 catalysts at different positions along the catalytic reactor. During the ignition of the catalytic partial oxidation of methane, the catalyst reduced from the end to the beginning of the catalyst bed and oxidized again...

Oscillatory Behavior during the Catalytic Partial Oxidation of Methane: Following Dynamic Structural Changes of Palladium Using the QEXAFS Technique