Since 71% of the earth's surface is covered by the sea, seawater desalination plays a pivotal role in addressing the water crisis. Membrane separation technologies, including reverse osmosis, electrodialysis, forward osmosis, pervaporation and membrane capacitive deionization, have been the recent focus for many research studies because of their simplicity and relatively low energy cost in comparison to the thermal driven distillation processes. Nanotechnology has opened a window for researching new nanomaterials which enhance desalination performance in an economical and sustainable manner. Experimental synthesis of nanomaterials with optimized desalination performance is a trial and error process, requiring considerable resources and time.Molecular dynamics (MD) simulation is an efficient method in investigating the transport behaviours at the nanoscale and thus provides a powerful tool for the design and performance analysis of graphene (GE)-based thin films. This Ph.D. thesis research aims to investigate the seawater desalination performance in capacitive deionization, FO, electronanofiltration and PV systems by adopting four GE-based nanostructures, namely, corrugated GE layers, stacked GE sheets, ionized graphene oxide (GO) layers and GO/metal organic framework (MOF) nanocomposite, via MD simulation.The surface corrugation of GE can modify its electronic, optical, mechanical and chemical properties. The seawater desalination performance through the corrugated GE nanochannel via capacitive deionization process is studied. The simulation results reveal that the corrugation of GE sheets greatly enhances the ion adsorption capacity, while adversely affecting the water flow rate in a capacitive deionization system. The strong anchoring effect existing in the regions which are bounded by crests and troughs of the upper and lower GE layers, respectively is identified to be responsible for the enhanced
Abstractxviii ion removal capacity. Moreover, desalination performance of such a system depends on the entrance configuration with its entrance effect becoming more significant at a higher electric field intensity.The stacked GE membrane performance greatly depends on the membrane structural parameters such as pore size (i.e., nanoslit width), pore offset, interlayer distance and number of GE layers. The complete rejection of ions is observed in the bilayer GE laminates, as a forward osmosis membrane, for the nanoslit widths less than 9 Å. The bilayer GE membrane can accomplish a complete ion rejection and maintain a higher water flux even at a nanoslit width larger than 9 Å, when an optimum interlayer distance of 8 Å and a completely misaligned pore configurations are adopted. Overall, the GE membranes in a forward osmosis system yield a low water flux but an enhanced ion retention capability in comparison to the GE membranes in a reverse osmosis system.Ionization of the functional groups such as the carboxylic acid of a GO sheet introduces a negative charge on the membrane surface and the desalination performance t...