Synergistic enhancement of <scp> CO ₂ </scp> capture from coal‐fired power plants by the ionic liquid and deep eutectic solvent

Abstract This study evaluates ionic liquids (ILs), deep eutectic solvents (DESs), and their hybrid systems using an integrated framework combining molecular screening, quantum analysis, and process simulation for post‐combustion CO 2 capture. A total of 300 DESs and 1122 ILs were screened using COSMO‐RS based on infinite dilution selectivity, followed by toxicity assessment via quantitative structure‐activity relationship. 1,3‐Dimethylimidazolium and Betaine:Malic acid (3:1) were identified as promising candidates with high CO 2 affinity and low toxicity. Quantum chemical analysis indicates that solvent‐CO 2 interactions are dominated by van der Waals forces, with interaction strength following IL &gt; IL+DES &gt; DES. Aspen Plus simulations show that IL and hybrid IL+DES systems outperform benchmark DES and conventional Monoethanolamine (MEA), achieving higher CO 2 recovery and purity while reducing solvent circulation and energy demand. Notably, thermal energy consumption decreases by up to 29% compared with MEA with negligible solvent loss, highlighting the potential of IL‐DES hybrid solvents for energy‐efficient CO 2 capture.