Reaction mechanism in non-thermal plasma enabled methane conversion: correlation between optical emission spectroscopy and gaseous products

Abstract

In this work, the reaction mechanism in non-thermal plasma enabled methane conversion driven by different sources, i.e. microwave discharge, nanosecond pulsed dielectric barrier discharge, and spark discharge, is investigated. The behaviour of reactive species is monitored using the optical emission spectroscopy (OES), while the final gaseous products are analysed with gas-chromatograph. A zero-dimensional (0D) reaction kinetics model is established to reveal the underlying reaction processes. By changing pressure, different plasma modes (diffuse and filamentary) are achieved and the relative emission intensity of different species and distribution of gaseous productions are manipulated. It is found that there is a strong correlation between the intensity-ratio of C2 A → X and CH A → X, gas temperature, and the relative concentration of C2 products in different discharge forms, i.e. higher intensity ratio of C2/CH is associated with higher gas temperature and more unsaturated hydrocarbon products. Assisted with the 0D reaction kinetics model, the relationship between the intermediate species and final products is illustrated. Based on the investigation in this work, it is proposed that intensity ratio of OES can be widely adapted as a non-intrusive and real-time process monitoring in the plasma-enabled methane conversion.