The design, synthesis, and characterization of aminosilica adsorbents for CO2 capture from dilute sources

The use of novel hyperbranched aminosilica (HAS) materials created through the ring-opening polymerization of aziridine from mesoporous silica supports was proposed for the adsorption of CO2 from dilute sources. The limits of the adsorptive performance of these adsorbents were investigated via the preparation of sets of materials with a range of aminopolymer loadings on several different silica supports with different pore space characteristics. Relationships were determined between the materials' amine loadings and the CO2 adsorption performance. Adsorbents with substantial remaining pore volume displayed universal adsorption kinetics when normalized by amine loading. However, materials with blocked pores displayed substantially slower adsorption kinetics due to hindered mass transfer. In both humid and dry conditions, the HAS adsorbent was found to have a surprisingly large CO2 capacity in light of the 250-fold reduction in CO2 partial pressure from 10% CO2 (flue gas application) to 400 ppm CO2 (air capture application). Finally, a new series of linear aminosilicas was created through the reaction of existing aminosilicas with N-protected-aziridines. Specifically, reaction of aminosilane-functionalized silicas with N-methylaziridine resulted in the linear growth of methylaminoethyl groups, effectively increasing the amine loading of the adsorbent by a stoichiometric amount of an additional amine per attached silane.PhDCommittee Chair: Jones, Christopher; Committee Member: Chance, Ronald; Committee Member: Koros, William; Committee Member: Sholl, David; Committee Member: Soper, Jak