Objective Molten catalytic methane pyrolysis coupled with chemical looping combustion technology was developed, and natural gas was used as material gas. It can produce hydrogen along with power generation and solid carbon.

Methods The process was simulated by Aspen Plus, and techno-economic feasibility in terms of economic benefits was analysed. The main influencing factors of methane conversion rate, pyrolysis reaction temperature, and PSA separation efficiency were discussed.

Results When the feedstock was 600 kmol/h, the system could produce 956 kmol/h hydrogen and 503 kmol/h solid carbon, and the system generating capacity was 9.43 MW. The CO₂ capture amount was 208 kmol/h while the capture ratio was 99.75%. The system performance was examined, and the results showed that the total system efficiency was 77.044%, wherein the hydrogen efficiency was 41.059%, the rate of solid carbon production was 31.453%, and the electricity efficiency was 4.532%.

Conclusion It was concluded that improving methane conversion and PSA efficiency, and reducing thermal cracking reaction temperature were significantly helpful in increasing product yield and total system efficiency.