Investigation of Ni catalyst activation during plasma-assisted methane oxidation

Atmospheric pressure plasma has shown promise in improving thermally activated catalytic reactions through a process termed plasma-catalysis synergy. In this work, we investigated atmospheric pressure plasma jet (APPJ)-assisted CH4 oxidation over a Ni/SiO2.Al2O3 catalyst. Downstream gas-phase products from CH4 conversion were quantified by Fourier transform infrared spectroscopy (FTIR). The catalyst near-surface region was characterized by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The catalyst was observed to be activated at elevated temperature (500 °C) if it was exposed to the APPJ operated at large plasma power. “Catalyst activation” signifies that the purely thermal conversion of CH4 using catalysts which had been pre-exposed to plasma became more intense and produced consistently CO product, even if the plasma was extinguished. Without the application of the APPJ to the Ni catalyst surface this was not observed at 500 °C. The study of different exposure conditions of the activated catalyst indicates that the reduction of the catalyst by the APPJ is likely the cause of the catalyst activation. We also observed a systematic shift of the vibrational frequency of adsorbed CO on Ni catalyst when plasma operating conditions and catalyst temperatures were varied and discussed possible explanations for the observed changes. This work provides insights into the plasma-catalyst interaction, especially catalyst modification in the plasma catalysis process, and potentially demonstrates the possibility of utilizing the surface CO as a local probe to understand the plasma-catalyst interaction and shed light on the complexity of plasma catalysis.