Methane conversion under cold plasma over Pd-containing ionic liquids immobilized on γ-Al2O3

Abstract

Pd-containing ionic liquid (IL) l-hexyl-3-methylimidazolium tetrafluoroborate (C6MIMBF4) immobilized on γ-Al2O3 (Pd-IL/γ-Al2O3) was prepared and characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and Brunauer-Emmett-Teller (BET) analysis. The influences of C6MIMBF4 loading and Pd on methane conversion to C2 hydrocarbons under cold plasma were investigated. FTIR and SEM analyses indicated that C6MIMBF4 had been successfully immobilized on γ-Al2O3 and the C6MIMBF4 showed excellent stability under cold plasma. The results of BET and methane conversion showed that with the increase in immobilization amount of C6MIMBF4 onto γ-Al2O3, the specific surface area and pore volume of IL/γ-Al2O3 decreased, while the selectivity and yield of C2 hydrocarbons increased. The selectivity of C2 hydrocarbons was 94.6% when the loading of C6MIMBF4 was 40%, and the percentage of C2H4 in C2 hydrocarbons was as high as 64% when using Pd-IL/γ-Al2O3 as a catalyst with no conventional thermal reduction treatment. Optical emission spectra (OES) from the cold plasma reactor during methane conversion were also studied. The results indicated that the intensity of the C2, CH, H, and C active species from methane and hydrogen decomposition increased when IL/γ-Al2O3 or Pd-IL/γ-Al2O3 was introduced into the plasma system. Based on the analyses of the gas product and OES spectra, it can be concluded that the surface catalyzed reactions between plasma and ionic liquid were very important for the reduction of Pd2+ and the formation of C2H4