Plasma-based dry reforming: improving the conversion and energy efficiency in a dielectric barrier discharge

Abstract

Dry reforming of methane has gained significant interest over the years. A novel reforming technique with great potential is plasma technology. One of its drawbacks, however, is energy consumption. Therefore, we performed an extensive computational study, supported by experiments, aiming to identify the influence of the operating parameters (gas mixture, power, residence time and “frequency”) of a dielectric barrier discharge plasma on the conversion and energy efficiency, and to investigate which of these parameters lead to the most promising results and whether these are eventually sufficient for industrial implementation. The best results, in terms of both energy efficiency and conversion, are obtained at a specific energy input (SEI) of 100 J cm⁻³, a 10–90 CH₄–CO₂ ratio, 10 Hz, a residence time of 1 ms, resulting in a total conversion of 84% and an energy efficiency of 8.5%. In general, increasing the CO₂ content in the gas mixture leads to a higher conversion and energy efficiency. The SEI couples the effect of the power and residence time, and increasing the SEI always results in a higher conversion, but somewhat lower energy efficiencies. The effect of the frequency is more complicated: we observed that the product of frequency (f) and residence time (τ), being a measure for the total number of micro-discharge filaments which the gas molecules experience when passing through the reactor, was critical. For most cases, a higher number of filaments yields higher values for conversion and energy efficiency. To benchmark our model predictions, we also give an overview of measured conversions and energy efficiencies reported in the literature, to indicate the potential for improvement compared to the state-of-the art. Finally, we identify the limitations as well as the benefits and future possibilities of plasma technology.