TY - GEN A1 - Baena-Moreno, Francisco Manuel A1 - González-Castaño, Miriam A1 - Navarro de Miguel, Juan Carlos A1 - Miah, Kamal Uddin Mohammad A1 - Ossenbrink, Ralf A1 - Odriozola, José Antonio A1 - Arellano-García, Harvey T1 - Stepping toward Efficient Microreactors for CO2 Methanation: 3D Printed Gyroid Geometry T2 - ACS Sustainable Chemistry & Engineering N2 - This work presents a comparative study towards the development of efficient micro-reactors based on 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, 0.5%Ru–15%Ni/MgAl2O4 catalyst is wash coated over two different micro-monolithic metal substrates: a conventional parallel channel honeycomb structure and a novel 3D-printed structure with a complex gyroid geometry. The effect of the metal substrate geometry is analyzed for several CO2 sources including ideal flue gas atmospheres, 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 at the best-case scenario a 14% improvement of CO2 conversion. Moreover, this contribution shows that systematically tailoring geometrical features of structured catalysts becomes an effective strategy to achieve improved catalysts 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 diffusional controlled regimes. KW - CO2 methanation KW - gyroid geometry KW - CH4 selectivity KW - gyroid-3D complex Y1 - 2021 U6 - https://doi.org/10.1021/acssuschemeng.1c01980 SN - 2168-0485 VL - 9 IS - 24 SP - 8198 EP - 8206 ER - TY - GEN A1 - González-Castaño, Miriam A1 - Baena-Moreno, Francisco Manuel A1 - Navarro de Miguel, Juan Carlos A1 - Miah, Kamal Uddin Mohammad A1 - Arroyo-Torralvo, Fátima A1 - Ossenbrink, Ralf A1 - Odriozola, José Antonio A1 - Benzinger, Walther A1 - Hensel, Andreas A1 - Wenka, Achim A1 - Arellano-García, Harvey T1 - 3D-printed structured catalysts for CO2 methanation reaction: Advancing of gyroid-based geometries T2 - Energy Conversion and Management N2 - This work investigates the CO2 methanation rate of structured catalysts by tuning the geometry of 3D-printed metal Fluid Guiding Elements (FGEs) structures based on periodically variable pseudo-gyroid geometries. The enhanced performance showed by the structured catalytic systems is mostly associated with the capability of the FGEs substrate geometries for efficient heat usages. Thus, variations on the channels diameter resulted in ca. 25% greater CO2 conversions values at intermediate temperature ranges. The highest void fraction evidenced in the best performing catalyst (3D-1) favored the radial heat transfer and resulted in significantly enhanced catalytic activity, achieving close to equilibrium (75%) conversions at 400 ◦C and 120 mL/min. For the 3D-1 catalyst, a mathematical model based on an experimental design was developed thus enabling the estimation of its behavior as a function of temperature, spatial velocity, hydrogen to carbon dioxide (H2/CO2) ratio, and inlet CO2 concentration. Its optimal operating conditions were established under 3 different scenarios: 1) no restrictions, 2) minimum H2:CO2 ratios, and 3) minimum temperatures and H2/CO2 ratio. For instance, for the lattest scenario, the best CO2 methanation conditions require operating at 431 ◦C, 200 mL/min, H2/CO2 = 3 M ratio, and inlet CO2 concentration = 10 %. KW - 3D-printing KW - Triply periodic minimal surfaces KW - Fluid guiding elements KW - CO2 methanation KW - Structured catalysts KW - Experiment design Y1 - 2022 U6 - https://doi.org/10.1016/j.enconman.2022.115464 SN - 2590-1745 VL - 258 ER -