Catalysis Today, Vol.362, 11-21, 2021
Methane Dry Reforming over Ni/Al2O3 Catalyst in Spark Plasma Reactor: Linking Computational Fluid Dynamics (CFD) with Reaction Kinetic Modelling
Efficient processes are needed for the valorisation of major greenhouse gases, methane and carbon dioxide, and electrification and energy storage are highly desired as well. Plasma based dry reforming provides the answer in all areas, as fast switch-on and-off times could use excess grid electricity to produce valuable products and decrease the carbon footprint. The reaction was studied in a non-equilibrium atmospheric pressure spark discharge reactor, which achieves higher yields than DBD reactors. CH4 and CO2 feed mixture at different ratios was converted to H-2 and CO with high selectivity, achieving conversions of 85% for CH4 and 75% for CO2. The syngas production energy cost was 315 kJ/mol, indicating 20% of input energy transferred to chemical energy. CO2 plasma regeneration and cyclic reaction operation was proposed to tackle the coking problem. With the intent of improving the yield, gaseous plasma was coupled with a solid Ni/Al2O3 heterogeneous catalyst, wash-coated on porous alumina foam material. The effects of specific energy input, external heating temperature and gas flow rate were also screened. In addition, a CFD and chemical kinetics model was developed in order to further investigate the system, which achieved good agreement with the experiments using relatively simple chemistry.