Conversion mechanism of thermal plasma-enhanced CH4-CO2 reforming system to syngas under the non-catalytic conditions

Thermal plasma activation of CH4-CO2 reforming (CRM) to syngas under non-catalytic conditions is an efficient and clean technology for the large-scale utilization of hydrocarbon resources and the conversion of greenhouse gases. This study investigates the equilibrium state and transformation mechanism of a CRM reaction system activated by thermal plasma through experimental, thermodynamic, and kinetic analyses. The experimental results illustrated that the CO2 conversion rate and H2 selectivity showed a downward trend with an increase in the CO2/CH4 molar ratio, whereas the CH4 conversion rate and CO selectivity showed the opposite trend. When CO2/CH4 molar ratio was 6/4, the selectivity for CO and H2 increased to 87.0 % and 80.8%, respectively. Excess CO2 promotes the partial oxidation of CH4 to eliminate carbon deposition, resulting in an H2/CO molar ratio value closer to 1. Thermodynamic results show that the thermal-plasma-initiated CRM reaction can reach thermodynamic equilibrium more easily than the conventional catalyzed reactions, achieving much higher feedstock gas conversion without carbon deposition. The kinetic results obtained from the PSR model revealed that CH4 and CO2 were cleaved to form free radicals at the instant of contact with the plasma flame. O, H, and other particles generated in the form of free radicals rapidly collided with each other and transformed into CO and H2, accelerating the reaction process. The results presented in this study will help reveal the transformation mechanism of the CRM reaction activated by thermal plasma under non-catalytic con-ditions and provide a new perspective for studying CRM reactions.

Automated summary

Thermal plasma activation of CH4-CO2 reforming is an efficient and clean technology for utilizing hydrocarbon resources and reducing greenhouse gases. This study investigates the equilibrium state and transformation mechanism of the reaction using experimental, thermodynamic, and kinetic analyses. The results show that the CO2 conversion rate and H2 selectivity decrease with increasing CO2/CH4 ratio, while the CH4 conversion rate and CO selectivity show the opposite trend. Excess CO2 promotes the partial oxidation of CH4, eliminating carbon deposition and achieving higher gas conversion without carbon deposition.