Abstract

Two silica-based nanomaterials, SBA15 and HMS, were modifed via surface impregnation with ternary Natural Deep Eutectic Solvents (NADES) composed of choline chloride, glycerol, and urea in varying molar proportions. A design of experiments (DoE) methodology was employed to optimize the NADES composition. The efects on the porous structure and CO2 adsorption capacity of the nanomaterials were evaluated using FTIR, TGA, N2 adsorption/desorption isotherms, TEM, and SAXS, both before and after impregnation. These analyses confrmed the successful incorporation of NADES onto the nanomaterials' surfaces while preserving their porous structure, pore size distribution, and surface area. Functionalization enhanced CO2 uptake, achieving 40.0 mg g−1 for SBA-15 impregnated at 15 wt% and 48.8 mg g−1 for HMS impregnated at 5 wt%, corresponding to increases of 17.4% and 25.2%, respectively. CO2 adsorption mechanisms were investigated through gravimetry, FTIR, TGA, NMR, and CO2 isotherms, revealing both physical adsorption via the nanomaterials’ surface area and chemical adsorption through carbamate/bicarbonate formation from amine and hydroxyl groups interacting with CO2. The isosteric heat of adsorption ranged from 22.7 to 32.5 kJ mol−1 also confrmed these adsorption mechanisms. The nano-materials exhibited stable adsorption capacity over fve adsorption–desorption cycles, with a slight decrease in CO2 uptake. However, heating to 100 °C restored the original weight, indicating efective CO2 desorption during each cycle.