Multicomponent gas separation and purification using advanced 2D carbonaceous nanomaterials

Multicomponent gas separation and purification is an important pre- or post-processing step in industry. Herein, we employed a multiscale computational approach to investigate the possibility of multicomponent low-weight gas (H₂, O₂, N₂, CO₂, CH₄) separation and purification using novel porous 2D carbonaceous nanomaterials, namely Graphdiyne (GD), Graphenylene (GN), and Rhombic-Graphyne (RG). The dispersion-corrected plane-wave density functional theory (DFT) calculation combined with the Climbing Image Nudged Elastic Band (CI-NEB) method was employed to study the gas/membrane interaction energy and diffusion barrier of different gases passing through the geometrically optimized membranes. The results from CI-NEB calculations were then fitted to the Morse potential function to construct a bridge between quantum mechanics calculations and non-equilibrium molecular dynamics (NEMD) simulation. The selectivity of each membrane for all binary mixtures was calculated using the estimated diffusion energy barriers based on the Arrhenius equation. Finally, a series of extensive NEMD simulations were carried out to evaluate the real word and time dependent separation process. According to the results, CH₄ molecules can be completely separated from the other gases using a GD membrane, O₂ molecules from CH₄, N₂, and CO₂ by a GN membrane, and H₂ molecules from all other gases using a RG membrane.