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STructured unconventional reactors for CO2-fRee Methane catalytic crackING

Periodic Reporting for period 1 - STORMING (STructured unconventional reactors for CO2-fRee Methane catalytic crackING)

Reporting period: 2022-09-01 to 2024-02-29

H2 will contribute to the decarbonization of hard-to-abate sectors such as the chemical industry, glass, tiles, and steel manufacturing as well as freight transport. The production of economic H2 by a low CO2 emissions (the notorious greenhouse gas) process is a requisite.
STORMING is developing a catalytic process showing zero CO2 emissions. The biomethane from biogas is converted through a process powered by renewable electricity into pure H2 and highly valuable carbon nanotubes (CNTs) for battery applications.
Low cost, easily available and non-toxic iron-based innovative catalysts, and the electrification (joule, microwave, and induction heating) of 3D printed structured reactors are investigated to enable an accurate thermal control resulting in high energy efficiency.
The work has been focused on the smart rational catalyst design proposed in STORMING. This methodology combines modelling (computational simulations by high throughput density functional, DFT, and model catalysts) with experimental results from laboratory catalytic reactors and in situ/operando synchrotron characterization. A combination of Fe-based promoted catalysts and reaction conditions have been identified to simultaneously produce H2 and base grow CNTs. The key species and mechanisms involved in the CH4 activation and CNTs growth have been identified.
The environmentally friendly and economical process development is supported by Life Cycle Assessment (LCA) of the laboratory process and market analysis of H2 and CNTs production and a preliminary techno economical analysis.
The development of the electrified catalytic reactors has started with the production of the first 3D printed monoliths and the setup of Joule and MW heated reactors. The kinetic and micro-kinetic modelling of the CNTs growth and Computational Fluid Dynamics (CFD) simulations is helping in the reactor design. Meanwhile the purification technologies of the biogas and the H2 produced have been selected.
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. The structuration of the catalyst by 3D printing confirmed the ability of the structured catalysts 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.