Mingsheng Luo

In this work, the efficient CO2 capture performance of functional deep eutectic solvents (DESs) as novel absorbents was systematically investigated via a combination of experimental measurements and molecular-scale computational methods. Ternary DESs were prepared by tuning the molar ratios of choline chloride (ChCl), monoethanolamine (MEA), and n-methyldiethanolamine (MDEA), and the effects of ChCl-MEA-MDEA composition, temperature, and regeneration performance were systematically studied during absorption-desorption cycles. Results suggest that the synthesized ternary DESs shows good thermal stability, with ChCl‐MEA‐MDEA (1:6:1) demonstrating excellent absorption performance, reaching 0.254 g CO2 g-1DES at 303.15 K. Furthermore, we found that desorption efficiency is significantly influenced by the MDEA content, with a regeneration efficiency of 93.7 % retained after five consecutive cycles. Besides, the results confirm the CO2 molecular reacts with amine groups to yield carbamate species by connecting spectroscopic analyses (FT-IR and NMR) and theoretical calculations (DFT and MD). Moreover, the results highlight that the identity of the hydrogen bond donor (HBD) is pivotal in optimizing DESs performance.