Design of Graphene/Ionic Liquid Composites for Carbon Capture

Pore size is a crucial factor impacting gas separation in porous separation materials, but how to control the pore size to optimize the separation performance remains a challenge. Here, we propose a design of graphene/ionic liquid composites with tunable slit pore sizes, where cations and anions of ionic liquids are intercalated between graphene layers. By varying the sizes of the ions, we show from first-principles density functional theory calculations that the accessible pore size can be tuned from 3.4 to 6.0 Å. Grand canonical Monte Carlo simulations of gas sorption find that the composite materials possess high CO₂ uptake at room temperature and 1 bar (up to ∼8.5 mmol/g). Further simulations of the sorption of gas mixtures reveal that high CO₂/N₂ and CO₂/CH₄ adsorption selectivities can be obtained when the accessible pore size is <5 Å. This work suggests a new strategy to achieve tunable pore sizes via the graphene/IL composites for highly selective CO₂/N₂ and CO₂/CH₄ adsorption.