Numerical Investigation of Carbon-catalyzed Methane Splitting for CO2-free Hydrogen Production

Hydrogen production through thermocatalytic methane decomposition (TMD) has emerged as a highly promising CO2-free pathway for sustainable hydrogen generation, overcoming the intrinsic carbon emissions associated with conventional reforming technologies. Nevertheless, the accurate assessment of the catalytic activity of carbonaceous species formed in situ during methane cracking still represents a major scientific and technological challenge. In this work, a comprehensive numerical methodology was developed for the processing and interpretation of experimental kinetic data obtained during methane thermocatalytic decomposition over carbon-based catalytic systems. The proposed approach enables the quantitative identification of the intrinsic catalytic contribution of evolving carbonaceous structures, whose physicochemical properties progressively change as a consequence of surface reconstruction phenomena, porosity evolution, and metal–support interactions. The methodology was subsequently validated and scaled up on a pilot-scale TMD unit, establishing a direct correlation between laboratory-scale kinetic behavior and industrially relevant operating conditions. Experimental data were integrated into a dedicated computational platform capable of simulating reaction kinetics, thermal transport phenomena, and reactor dynamics under variable thermal regimes and reactor configurations. The developed software tool provides an advanced decision-support framework for process intensification and optimization, enabling predictive evaluation of hydrogen productivity, carbon morphology evolution, and overall energy efficiency. The present study contributes both to the fundamental understanding of carbon-mediated catalytic mechanisms and to the digitalization of TMD reactor engineering, thereby supporting the future deployment of high-efficiency and low-emission hydrogen production technologies.