Access to clean water is one of the world's greatest concerns. Because 97% of global water resources are seawater, desalination via reverse osmosis (RO) membrane process has become a vital technology to obtain drinkable water. At the same time, the discharge of industrial waste effluents containing heavy metal ions to the available water resources (seawater and brackish water) without adequate pre-treatment is a major cause of water pollution. Heavy metal rejection using nanofiltration (NF) membrane process is a recognized water treatment methodology. Thin-film nanocomposite (TFN) membranes have shown vast performance enhancement using both RO and NF processes. However, TFN membrane fabrication has been limited due to poor dispersion of the nanoparticles in the polyamide (PA) layer of the membrane, and the leaching of the often-hazardous nanoparticles from the TFN membranes. For various reasons such as their dispersibility in aqueous media, safety, high aspect ratio, and functionality, cellulose nanocrystals (CNCs) are an ideal nanoparticle for inclusion in TFN membranes. Because of their hydrophilicity, CNCs have more commonly been dispersed in the aqueous monomer solution during PA interfacial polymerization. In this thesis, we investigated two different CNC modification routes to improve CNC dispersion within the trimesoyl chloride (TMC)/n-hexane (non-aqueous) monomer solution. In one case, we acetylated the CNCs (ACNCs) using a straightforward, efficient, solvent-free method to achieve a more uniform CNC dispersion in the PA layer. The resulting ACNCs were less hydrophilic, which allowed increased nanoparticle loading and improved dispersion in the PA layer. In an RO desalination process, compared to unmodified CNC-TFN membranes, the NaCl rejection of the ACNC-TFN membranes remained stable (at 98-99%) up to a 0.4 wt% loading, while water permeability increased by up to 40%. For the second case, we synthesized L-cysteine functionalized CNCs (CysCNCs) and incorporated them into the PA layer for testing in an NF wastewater treatment process. The amine functional groups of L-cysteine covalently bonded with the acyl chloride groups of the TMC monomer. This resulted in improved nanoparticle dispersion but could also have prevented nanoparticle leaching. Moreover, because L-cysteine contains strong chelating groups, their inclusion in the PA layer led to improved heavy metal rejection. A loading of 0.1 wt% CysCNCs in the TFN membranes provided high rejection of both copper and lead ions, 98.1 and 95.2%, respectively. The CysCNCs were also evaluated in an NF desalination process resulting in a 40% increase in water permeability with almost no decline in Na₂SO₄ (97-98%), MgCl₂ and NaCl rejection. The modified CNCs enabled us to overcome the water permeability/selectivity trade-off in CNC-TFN membranes for both RO and NF membrane desalination. Finally, we developed an experimental protocol to investigate the effect of the adsorption of heavy metal ions (if any) on the performance of thin film composite (TFC) and TFN membranes in NF. We confirmed that adsorption occurred, and the equilibrium capacity of the membranes was reached after 8 - 12 h of the experiment. Despite reaching the equilibrium capacity, the water permeability and heavy metal rejection remained at their highest values. This led to the conclusion that the adsorbed heavy metals altered the membrane surface, thereby improving the performance of both TFC and TFN membranes. The ability to modify CNCs enables one to achieve a controlled range of hydrophilicity/ hydrophobicity. This allows one to fine-tune CNC compatibility with the TMC/n-hexane non-aqueous monomer solution and enable improved dispersion in the PA layer, eventually leading to improved TFN membrane performance for both RO and NF processes.

Thin film Nanocomposite (TFN) membranes are a relatively new class of high-performance semipermeable membranes for Reverse Osmosis (RO) applications. Large scale applications of TFN membranes have not been achieved yet due to the high production cost of the nanoparticles, agglomeration of the nanoparticles in the thin polyamide matrix of the membrane, and leaching out of typically toxic inorganic nanoparticles into the downstream. In this work, these challenges are addressed by incorporation of two different nanofillers: Cellulose NanoCrystals (CNC), and surface functionalized Halloysite NanoTubes (HNT). Amine groups, carboxylic acid groups, and the first generation of poly(amidoamine) (PAMAM) dendrimers were used for functionalization of the HNT. CNC and HNT are environmentally friendly, low/non-toxic, abundant, and inexpensive nanoparticles with a unique size, and chemical properties. TFN membranes were synthesized via in situ interfacial polymerization of m-phenylenediamine (MPD) with trimesoyl chloride (TMC) and the nanoparticles. The control Thin Film Composite (TFC) membranes, and CNC and HNT based TFN membranes were characterized by Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-Ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), Fourier Transform Infrared spectroscopy (FTIR) and contact angle measurements. The antifouling capacity of CNC based membranes was investigated with a solution of Bovine Serum Albumin (BSA) as the fouling agent. Also, the leachability of the HNT from the membranes was examined by shaking the membranes in a batch incubator for 48 h, and then tracing the leached out HNT using Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Separation characteristics of the membranes were studied by desalination of synthetic brackish water with a cross flow RO filtration system. It was revealed that incorporation of functionalized HNT enhanced the permeate flux without sacrificing the salt rejection (99.1 % ± 0.1 %). Also, incorporation of 0.1% (w/v) CNC doubled the permeate flux (from 30 to 63 L/m2.h at 20 bar) without compromising the salt rejection (97.8%). At the same time, leaching out of HNT from the TFN membranes was decreased as a result of the HNT functionalization and formation of covalent bonds with the TMC. Also, antifouling properties of the CNC-TFN membranes were 11% improved in comparison with control TFC membrane.