Abstract
Semiclathrate hydrates of tetra-n-butylammonium fluoride (TBAF) are potential CO2 capture media because they can capture CO2 at near ambient temperature under moderate pressure such as below 1 MPa. In addition to other semiclathrate hydrates, CO2 capture properties of TBAF hydrates may vary with formation conditions such as aqueous composition and pressure because of their complex hydrate structures. In this study, we investigated CO2 capture properties of TBAF hydrates for simulated flue gas, that is, CO2 + N2 gas, by the gas separation test with three different parameters for each pressure and aqueous composition of TBAF in mass fraction (w TBAF). The CO2 capture amount in TBAF hydrates with w TBAF = 0.10 was smaller than that obtained with w TBAF = 0.20 and 0.30. The results found that gas pressure greatly changed the CO2 capture amount in TBAF hydrates, and the aqueous composition highly affected CO2 selectivity. The crystal morphology and single-crystal structure analyses suggested that polymorphism of TBAF hydrates with congruent aqueous solution may lower both the CO2 capture amount and selectivity. Our present results proposed that an aqueous solution with w TBAF = 0.20 is advantageous for the CO2 capture from flue gas compared to near congruent solutions of TBAF hydrates (w TBAF = 0.30) and dilute solution (w TBAF = 0.10).