Nanosecond Pulsed DBD for CH4 and CO2 Transformation into Value-added Chemicals: a Parametric Study
摘要
CH4 reforming with CO2 was investigated using nanosecond pulsed DBD plasma, focusing on pulse parameters (pulse width and repetition frequency), discharge power, residence time and molar ratios on reaction performance. Furthermore, the impact of oxygen addition to the feed gas mixture was evaluated. At a constant power of 16 W and flow rate of 40 ml. min-1, the increase in pulse width from 150 ns to 175 ns enhanced CH4 conversion from 18.6 to 21.1%, while CO2 conversion remained relatively stable, around 8.0%. Notably, the selectivity of products remained constant despite these changes, the main product being CO with a selectivity close to 50%. Increasing the frequency resulted in improved conversions, with optimal CO2 and CH4 conversions of 8.0% and 21.1%, respectively at 10 kHz. Methanol was identified with a low selectivity of 1.8% at 10 kHz. By varying the oxygen percentage, a marked shift in product selectivity from hydrocarbons to CO was observed. At 20% oxygen content in the feed gas, a CO selectivity of nearly 85% was achieved, with a methane conversion of 33.1%. Nanosecond pulsed plasma discharge with O2 favors the partial oxidation of methane. A study of the effect of residence time revealed significant differences in reaction pathways between oxygen-free and oxygen-containing mixtures. Without oxygen, propane emerges as a primary reaction product when using a pure mixture of CH4 and CO2. However, when oxygen is present, the formation pathway for propane changes, with ethane serving as an intermediate. To our knowledge, this has never been reported in the literature.