H2 and carbon production from CH4 decomposition and regeneration based on Fe/CaO-Ca12 Al14 O33 catalyst looping cycles

Catalytic decomposition of CH4 is a prospective method to produce high-purity H2 without COx. Fe-based catalysts possess the advantages of low cost and non-toxicity. In this work, the Fe/CaO-Ca12Al14O33 catalyst was firstly used in catalytic decomposition of CH4/regeneration cycles. H2 and high-value solid carbon were obtained via catalytic decomposition of CH4/regeneration cycles. H2 from steam gasification of carbon deposition and CO2 from CaCO3 calcination were expected for methanol production. Characteristics of the Fe/CaO-Ca12Al14O33 catalyst for catalytic decomposition of CH4 and regeneration were investigated through a fixed-bed reactor. The highest average CH4 conversion of the Fe/CaO-Ca12Al14O33 catalyst is 86.03% with the H2 concentration over 92%. Abundant oxygen vacancies in the Fe/CaO-Ca12Al14O33 catalyst promote CH4 adsorption and electron transfer, which facilitates catalytic decomposition of CH4. In-situ capture of CO2 by CaO enhances H2 production from gasification with a maximum concentration of 82.07%. Ca12Al14O33 forms the skeletons of the materials, inhibiting sintering, agglomeration, and maintaining favorable pore structures. The average CH4 conversion of the Fe/CaO-Ca12Al14O33 catalyst is over 72.00% after 8 cycles. Wind power and solar power are expected to provide the constant energy source for the catalytic decomposition of CH4/regeneration process. The Fe/CaOCa12Al14O33 catalyst seems promising for H2 production via catalytic decomposition of CH4/regeneration cycles.