The origin of self-sustained reaction-rate oscillations in the oxidation of methane over nickel: an operando XRD and mass spectrometry study

The self-sustained kinetic oscillations in the catalytic oxidation of methane over Ni foil have been studied at atmospheric pressure using an X-ray diffraction technique and mass spectrometry. It has been shown that the regular reaction-rate oscillations appear under oxygen-deficient conditions and the period of oscillations varies between approximately 200 and 4000 s. The operando measurements have revealed a higher activity of metallic Ni in the reaction than NiO oxide and have unambiguously showed that the oscillations arise due to the reversible bulk oxidation of Ni to NiO.