Experimental testing and mechanism investigation of amine-functionalized layered vermiculite for CO2 capture

Solid amine adsorbents have attracted significant attention due to their low energy consumption, high selectivity, and environmental friendliness, positioning them as the most promising technology for CO2 capture. However, current adsorbent carrier materials commonly encounter challenges such as expensive costs and inadequate stability. In this study, acid-activated expanded vermiculite carrier (AEV) with a large pore volume and hierarchical pore structure was prepared. Subsequently, a series of functionalized polyethyleneimine (PEI) adsorbents were synthesized and employed in CO2 capture experiments to investigate the impact of PEI loading and temperature on adsorption characteristics. The results showed that the acid-modified expanded vermiculite with a large pore volume structure significantly increased amine loading, while the layered structure network promoted amine dispersion. Under the conditions of 50 wt% PEI loading, the CO2 capture capacity of AEV reached 3.29 mmol/L at 75 ℃. Furthermore, density functional theory was utilized to calculate the adsorption energy and Gibbs free energy change of CO2 and polyethyleneimine molecules. The HOMO and LUMO distributions of CO2 molecules with different polyethyleneimine chains were determined using frontier orbital theory, combined with infrared spectroscopy results confirming the conversion of CO2 into carbamate. Additionally, AEV-PEI50 adsorbent exhibited good stability during 8 cycles of the adsorption process. The obtained results demonstrate that the utilization of layered mesoporous scaffolds offers notable benefits in terms of efficient CO2 capture.