Simulation Insights for Graphene-Based Water Desalination Membranes

Molecular dynamics simulations were employed to study the transport of water and ions through pores created on the basal plane of one graphene sheet (GS). Graphene pore diameters ranged from 7.5 to 14.5 Å. Different pore functionalities were considered, obtained by tethering various functional groups to the terminal carbon atoms. The ease of ion and water translocation across the pores was monitored by calculating the potential of mean force along the direction perpendicular to the GS pore. The results indicate that effective ion exclusion can be achieved only using nonfunctionalized (pristine) pores of diameter ~7.5 Å, whereas the ions can easily penetrate pristine pores of diameters ~10.5 and 14.5 Å. Carboxyl functional groups can enhance ion exclusion for all pores considered, but the effect becomes less pronounced as both the ion concentration and the pore diameter increase. When compared to a carbon nanotube of similar pore diameter, our results suggest that GS pores functionalized with COO(-) groups are more effective in excluding Cl(-) ions from passing through the membrane. Our results suggest that narrow graphene pores functionalized with hydroxyl groups remain effective at excluding Cl(-) ions even at moderate solution ionic strength. The results presented could be useful for the design of water desalination membranes.