Multi-scale computational screening to accelerate discovery of IL/COF composites for CO2/N2 separation

Covalent organic frameworks (COFs) have emerged as novel adsorbents and membranes for gas separation. Incorporation of ionic liquids (ILs) into COFs is important to exceed the current performance limits COFs. However, synthesis testing a nearly unlimited number IL/COF combinations are simply impractical. Herein, we used multi-scale computational screening approach combining COnductor-like Screening MOdel Realistic Solvents (COSMO-RS) method, Grand Canonical Monte Carlo (GCMC), molecular dynamics (MD) simulations, density functional theory (DFT) calculations unlock both adsorption- membrane-based CO2/N2 separation performances composites. Several adsorbent membrane assessment metrics including selectivity, working capacity, regenerability, score, permeability were computed. Our results revealed that IL incorporation significantly improves adsorption selectivities (from 12 26) scores 3.7 mol/kg). By performing DFT calculations, nature interactions between CO2, N2, COFs, their IL-incorporated composites was evaluated. The high CO2 selectivity attributed cooperative intermolecular effects induced by COF IL. Finally, studied, showed they achieve higher permeabilities (2.4 × 104–9.4 105 Barrer) than polymeric zeolite with comparable (up 15.7). This shows great promise replace conventional materials flue will be useful in accelerating experimental efforts design new can high-performance