Combining Electrochemical CO2 Capture with Catalytic Dry Methane Reforming in a Single Reactor for Low-Cost Syngas Production

We here report a potentially low-cost catalytic dry methane reforming process to make syngas with CO2 electrochemically captured from a CO2 source via a mixed conducting membrane in a single reactor. The mixed conducting electrochemical membrane is a composite comprising an O2--conductor and molten carbonate phase, where the catalytic bed contains a Ni-MgO-1 wt % Pt (NMP) or LaNi0.6Fe0.4O3.delta (LNF) catalyst. The reactor with the NMP catalyst generally outperforms the LNF counterpart in CH4 conversion rate and syngas production yield. At 850 degrees C and over the NMP catalyst, the membrane reactor yields a CO2 permeation flux of 2.25 mL min(-1) cm(-2), a H-2 and CO production rate of 3.75 and 3.24 mL min(-1) cm(-2), respectively, and a CH4 conversion of 93.9%. The LNF catalyst shows a long activation period due to the slow Ni ex-solution process but does offer a better coking and coarsening resistance. Long-term stability tests show no apparent sign of degradation within 200 h. With 3% H2O added into methane, the reactor can produce a syngas with higher H-2/CO ratio preferable for liquid fuels synthesis. Overall, this work demonstrates the technical feasibility of a combined capture and conversion "all-in-one" CO2 reactor for dry reforming of CH4