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Electricity generation at nuclear power plants produces a large amount of high-level radioactive waste (HLW) every year, which has long-term detrimental effects on humans and the environment. Other applications of nuclear technology (e.g., medicine, research, nuclear weapons, industry) also produce radioactive waste (e.g., low-level radioactive waste, LLW, Intermediate-level waste, ILW). The potential of deep geological repositories (DGRs) as an option for disposal of radioactive waste (HLW, ILW, LLW) has been examined in several countries, including Bulgaria, Canada, China, Finland, France, Germany, India, Japan, Russia, Spain, Sweden, Switzerland, Ukraine and the United Kingdom and are still under discussion. In Ontario, Canada, DGRs with a multi-barrier system comprised of a sedimentary rock formation (i.e., a natural barrier) and an engineered barrier system (EBS) are currently under consideration. An EBS consists of various components, such as waste containers, buffer, backfill, and tunnel sealing materials, intended to prevent the release of radionuclides. Several engineered barrier materials, including a mixture of bentonite and sand, are currently being considered for use in DGRs for nuclear waste in Ontario. Bentonite has some advantageous physical and chemical properties, such as low permeability, high plasticity, and high swelling potential, which provide it with a good sealing ability and thus make it an effective barrier. However, interaction between the compacted bentonite–sand mixture and underground water chemistry fluids (chemical factor) in the DGR could significantly alter the favourable properties of bentonite (e.g., swelling potential), thus influencing its performance when used in an EBS and eventually jeopardizing the overall safety of DGRs. In addition, other parameters, such as the clay content, initial dry density and moisture content of the compacted barrier (physical factors), as well as the presence of salts in groundwater may affect the physical and physiochemical properties of barrier materials. Moreover, during the lifetime of a DGR for used spent fuel, the bentonite–based barrier material will not only be exposed to a broad range of groundwaters with different chemical compositions, but also to high temperatures (heat generated by the nuclear wastes) (thermal factor). Thus, the interaction between the compacted bentonite–sand mixture, the surrounding groundwater and the heat from the nuclear waste material could jeopardize the favourable properties of the bentonite-based (bentonite-sand) barrier material. Properties of a bentonite-sand barrier is an important characteristic to study while designing and constructing an EBS for a DGR. Thus, to understand and assess the operations of DGRs in Ontario, comprehensive studies must be performed on engineering properties like swelling behaviour, permeability, and thermal conductivity. The goal of this research study is to experimentally investigate the physical, chemical and thermal factors that influencing the engineering properties of a barrier material made up of bentonite-sand composite used in DGRs for nuclear waste in Ontario. Compacted samples are subjected to one-dimensional free swell test to understand the swelling behaviour of the material. Hydraulic conductivity was investigated using a flexible wall permeability test. Thermal conductivity and diffusivity were tested using Decangon KD2 Pro with TR-1 and and KS-1 sensors. The specimens contain different bentonite–sand mixture ratios (20:80, 30:70, 50:50, and 70:30 dry mass), and they are tested under conditions with differing bentonite content, dry density, groundwater chemistry, and temperature. Additional tests were conducted to investigate the microstructure of the specimens. These tests include X-ray diffraction (XRD) analysis, mercury intrusion porosimetry (MIP), and thermogravimetric analyses (TG/DTG). The results reveal that the time and strain required to achieve maximum swelling of compacted bentonite–sand specimens increase with the increase of initial dry density. The simulated saline solutions of Guelph and Trenton groundwater are found to suppress the swelling of the bentonite–sand specimens. This in turn leads to the increase of hydraulic conductivity and decrease of thermal properties of the barrier material. However, the impact of the salinity is significantly reduced by increasing the dry densities and sand content of the compacted material. Moreover, the coupled effect of salinity and temperature decreases the swelling potential of the bentonite-sand mixture. Also, some transformation of Na-montmorillonite into Ca-Montmorillonite was observed. The results also indicate that some montmorillonites might have been transformed into illites, thereby further decreasing the swelling potential of the bentonite-based barrier.

Brittleness of a polymeric material has a direct relationship with the material's performance and furthermore shares an inverse relationship with that material's flexibility. The concept of flexibility of materials has been understood but merely explained with a hand-waving manner. Thus, it has never been defined by a calculation, thereby lacking the ability to determine a definite quantitative value for this characteristic. Herein, an equation is presented and proven which makes determining the value of flexibility possible. Such an equation could be used to predict a material's flexibility prior to testing it, thus saving money and valuable time for those in research and in industry. Substantiating evidence showing the relationship between flexibility of polymers and their respective mechanical properties is presented. Further relating the known tensile properties of a given polymer to its flexibility is expanded upon by proving its relationship to the linear coefficient of thermal expansion for each polymer. Additionally, determining flexibility for polymers whose chemical structures have been compromised by respective solvents has also been investigated to predict a solvent's impact on a polymer after exposure. Polymers examined through literature include polycarbonate (PC), polystyrene (PS), teflon (PTFE), styrene acrylonitrile (SAN), acrylonitrile butadiene styrene (ABS), poly(ethersulfone) (PES), low density polyethylene (LDPE), polypropylene (PP), poly(methyl methacrylate) (PMMA), and poly(vinylidene fluoride) (PVDF). Further testing and confirmation was made using PC, PS, ABS, LDPE, PP, and PMMA.

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With the aim of developing a deeper understanding of particle behaviour within nano-hybrid materials, this thesis investigates the particle-particle and particle-polymer interactions that influence and control cellulose nanocrystal dispersion in aqueous and non-aqueous environments. / Cellulose nanocrystals (CNCs) are rigid rod-shaped nanoparticles derived from bio-based resources and are considered an emerging nanomaterial based on their commercial availability and favourable properties. CNCs have great potential as reinforcing agents in hybrid materials and composite applications if they are well-dispersed. Whereas colloidal stability is effectively described by established theories, dispersing nanoparticles from an aggregated state, and their interaction with polymers can be difficult to predict and control. Herein, the particle-particle and particle-polymer interactions that govern CNC dispersibility in aqueous and non-aqueous environments are examined. The surface chemistry, morphology and colloidal/thermal stability of CNCs from North American industrial producers were extensively characterized such that particle interactions could be reproducibly measured from a known starting material. Industrially produced CNCs compared well to those produced at the bench-scale, implying that laboratory results should be translatable to the development of new CNC-based products. To examine particle-particle interactions within dry CNC aggregates, a surface plasmon resonance-based platform was developed to monitor CNC film swelling in a range of solvents and salt solutions. Water was observed to interrupt particle-particle hydrogen bonding most effectively, however film stability, and ultimately particle aggregation, was maintained by strong van der Waals interactions. Moreover, particle spacing and overall film thickness was found to be independent of the CNC surface chemistries and surface charge densities examined, yet the rate of film swelling scaled with the ionic strength of the surrounding media. Polyethylene glycol (PEG) was used as a model, non-ionic, water-soluble polymer to investigate polymer adsorption to CNC surfaces in water. PEG did not adsorb to CNCs despite the abundance of hydroxyl groups, which is in direct contrast to silica particles that are well known to hydrogen bond with PEG. Combining the knowledge of both particle-particle and particle-polymer interactions, PEG nanocomposites reinforced with CNCs and silica were compared and particle dispersibility was related to composite performance. Although PEG does not adsorb to CNCs in aqueous environments, polymer adsorption does occur in dry polymer nanocomposites leading to good dispersibility and improved mechanical properties. Overall, the work presented here yields new insight into the forces that govern CNC dispersion and provides a foundation from which a variety of new CNC-based products can be developed. / Thesis / Doctor of Philosophy (PhD) / Using particles derived from renewable resources to reinforce plastics and other materials has the potential to make products lighter, stronger and more environmentally friendly. However, to make these products we need to understand how to control and distribute particles uniformly throughout hybrid/composite materials. This work uses particles extracted from trees and cotton, known as cellulose nanocrystals, to reveal which factors govern particle dispersion in reinforced composite materials. To do so, first the properties and performance of commercially available cellulose nanocrystals were extensively analyzed and compared to form the basis from which interactions can be understood. Next, particle films were measured in water, organic solvents and salt solutions to better understand how aggregated cellulose nanocrystals can be separated within composite materials. The interactions between water-soluble polymers and cellulose nanocrystals were then investigated to reveal how polymer adsorption impacts particle dispersibility. Finally reinforced polymer composites were prepared with uniformly distributed cellulose nanocrystals and the crystallization and mechanical properties were investigated. By developing a deeper understanding of the factors that control cellulose nanocrystal dispersion we can learn how to make a variety of new and improved environmentally conscious products.