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Amines supported on porous solid materials have a high CO2 adsorption capacity and low regeneration temperature. However, the high amine load on such substrates and the substrate itself may lead to substantial pressure drop across the reactor. Herein, we compare the CO2 adsorption capacity and pressure drop of fumed silica powder to 3D-printed monolithic fumed silica structures, both functionalized by polyethylenimine (PEI), and find a drastically reduced pressure drop for 3D-printed substrates (0.01 bar vs. 0.76 bar) in the sorption bed with equal CO2 adsorption capacity. Furthermore, the effect of 3D-printing nozzle diameter and PEI loading on the adsorption capacity are investigated and the highest capacities (2.0 mmol/g at 25 °C with 5000 ppm CO2) are achieved with 0.4 mm nozzle size and 34 wt% PEI loading. These high capacities are achieved since the 3D printing and subsequent sintering (700 °C) of monolithic samples does not compromise the surface area of the fumed silica. Finally, the comparison between 3D-printed monoliths and extruded granulate of varying diameter reveals that the ordered channel system of 3D-printed structures is superior to randomly oriented granulate in terms of CO2 adsorption capacity. [ABSTRACT FROM AUTHOR]