2024-09-272024-09-272021-062168-0485https://hdl.handle.net/11441/162972This work presents a comparative study toward the development of efficient microreactors based on three-dimensional (3D)-printed structures. Thus, the study evaluates the influence of the metal substrate geometry on the performance of structured catalysts for the CO2 methanation reaction. For this purpose, the 0.5%Ru–15%Ni/MgAl2O4 catalyst is washcoated over two different micromonolithic metal substrates: a conventional parallel channel honeycomb structure and a novel 3D-printed structure with a complex gyroid geometry. The effect of metal substrate geometry is analyzed for several CO2 sources including ideal flue gas atmospheres and the presence of residual CH4 and CO in the flue gas, as well as simulated biogas sources. The advantages of the gyroid 3D complex geometries over the honeycomb structures are shown for all evaluated conditions, providing in the best-case scenario a 14% improvement in CO2 conversion. Moreover, this contribution shows that systematically tailoring geometrical features of structured catalysts becomes an effective strategy to achieve improved catalyst performances independent of the flue gas composition. By enhancing the transport processes and the gas–catalyst interactions, the employed gyroid 3D metal substrates enable boosted CO2 conversions and greater CH4 selectivity within diffusion-controlled regimes.application/pdf9 p.eng3D printingMicromonolithsCO2 methanationStructured catalystsSynthetic natural gas productioninfo:eu-repo/semantics/articleinfo:eu-repo/semantics/openAccess10.1021/acssuschemeng.1c01980