Plasma-catalytic hydrogenation of CO2 for the cogeneration of CO and CH4 in a dielectric barrier discharge reactor: effect of argon addition

Abstract

Plasma-catalytic CO2 hydrogenation over a Ni/Al2O3 catalyst for the cogeneration of CO and CH4 has been carried out in a dielectric barrier discharge (DBD) reactor at 150 °C. The presence of the Ni catalyst in the DBD reactor has clearly demonstrated a plasma-catalytic synergistic effect at low temperatures, as the reaction performance of the plasma-catalytic CO2 hydrogenation is significantly higher than that of the sum of the individual processes (plasma process and thermal catalytic process) at the same temperature. The addition of argon (up to 60%) in the reaction enhances the conversion of CO2, the yield of CO and CH4 and the energy efficiency of the plasma process. The formation of metastable argon (Ar*) in the plasma could create new reaction routes which make a significant contribution to the enhanced CO2 conversion and production of CO and CH4. The introduction of Ar decreases the breakdown voltage of the feed gas and promotes charge transfer through the reactor. In addition, we find that the selectivity of CO is almost independent of the Ar content in the feed gas, while increasing the Ar content from 0 to 60% enhances the CH4 selectivity by 85%. This phenomenon suggests that the presence of Ar* might promote the methanation of CO and CO2 with hydrogen at low temperatures. Moreover, the molar ratio of CO/CH4 in the plasma-catalytic hydrogenation of CO2 can also be controlled by changing the Ar content in the feed gas.