We have proposed, for the first time, base growth of CNTs on Fe-based catalysts under reaction conditions able to achieve H2 productivities above 5 LH2/gcat*h. The CNTs base growth has been demonstrated by ex situ and in situ characterization of real and model catalysts with techniques developed for this purpose. Meanwhile, the key role of the active phase on balancing the CH4 activation and C diffusion has been proved by computational and experimental studies, as well as the kinetic model. For the Induction heated reactor Fe–Ni–Co catalysts achieve the highest and most stable CH₄ conversion (> 40 %) and carbon yields (≈ 0.2 g h⁻¹) at 650 °C for more than 10 h, since they act as both magnetic susceptors and active catalytic phases.
The structuration of the catalyst by 3D printing confirmed the ability of the structured materials to decrease the reactor clogging and promote the Joule and MW heating.
These results are the basis for the further development of a continuous process in STORMING that will confirm the feasibility of the biomethane decomposition for the CO2-free production of H2, valorising the carbon as CNTs. Moreover, they will contribute to promote the research on cheap, easily available and non-toxic Fe-based catalysts. Last but not least, they provide a robust methodology for the development of other types of catalysts.