Experimental and DFT study of Na4SiO4 doped with oxysalts for high-temperature CO2 capture

Eutectic doping has been considered as one of the most efficient ways to modify the Na4SiO4-based CO2 sorbent. Nevertheless, the effects of different acid radical ions and alkali metal cations of the oxysalts on the CO2 capture performances of Na4SiO4 have never been explored. In this study, Na4SiO4-based CO2 sorbents were prepared using four kinds of oxysalts as the dopants. The effects of acid radical ions/alkali metal cations, doping ratios and sorption/desorption temperatures on the CO2 capture performances of sorbents were investigated. The results showed that the promotion effects of CO32− and Li+/K+ ions were stronger than others, the maximum CO2 sorption capacity of Na4SiO4-30Li2CO3 and Na4SiO4-30K2CO3 at 700 °C reached 20.6 wt% and 19.5 wt%, respectively. The cyclic sorption capacity of Na4SiO4-30Li2CO3 was 8.5 wt%, which was 40.0% higher than that of Na4SiO4. Further, the oxysalt dopants could enhance the CO2 adsorption energy on the Na4SiO4 surfaces and reduce the energy level of the systems using density functional theory calculation, which were consistent with the experimental values. Finally, the effects of water vapor on the sorption of Na4SiO4 and Na4SiO4-K2CO3 were simulated, which could enhance the activity of O atoms on sorbent surfaces and promote rapid carbonization during the sorption progress. Thus, Na4SiO4 doped with oxysalts exhibit promising potential for high-temperature CO2 capture application.