A Novel Process for Renewable Methane Production: Combining Direct Air Capture by K₂CO₃/Alumina Sorbent with CO₂ Methanation over Ru/Alumina Catalyst

CO₂ methanation over supported ruthenium catalysts is considered to be a promising process for carbon capture and utilization and power-to-gas technologies. In this work 4% Ru/Al₂O₃ catalyst was synthesized by impregnation of the support with an aqueous solution of Ru(OH)Cl₃, followed by liquid phase reduction using NaBH₄ and gas phase activation using the stoichiometric mixture of CO₂ and H₂ (1:4). Kinetics of CO₂ methanation reaction over the Ru/Al₂O₃ catalyst was studied in a perfectly mixed reactor at temperatures from 200 to 300 °C. The results showed that dependence of the specific activity of the catalyst on temperature followed the Arrhenius law. CO₂ conversion to methane was shown to depend on temperature, water vapor pressure and CO₂:H₂ ratio in the gas mixture. The Ru/Al₂O₃ catalyst was later tested together with the K₂CO₃/Al₂O₃ composite sorbent in the novel direct air capture/methanation process, which combined in one reactor consecutive steps of CO₂ adsorption from the air at room temperature and CO₂ desorption/methanation in H₂ flow at 300 or 350 °C. It was demonstrated that the amount of desorbed CO₂ was practically the same for both temperatures used, while the total conversion of carbon dioxide to methane was 94.2–94.6% at 300 °C and 96.1–96.5% at 350 °C.