Interest in microemulsions as potential platforms for polymerization stems from the wide range of phase behaviour dependant morphologies and domain sizes that can be generated in a low viscosity environment. By introducing polymerizable components into the oil and aqueous phases of a microemulsion, we may essentially create a low viscosity, low interfacial tension, bicontinuous template with nanostructured morphologies and narrow domain size distributions analogous to those generated through conventional interpenetrating polymer network (IPN) synthesis and spinodal decomposition. The main objective of this dissertation is to test the application of bicontinuous microemulsion templates to the formulation and polymerization of a silicone-hydrogel IPN. In addition, the project expands on the classical definition of IPNs to a scale of entanglement at the level of groups of polymer chains, as opposed to molecular or chain-level entanglement. This study is divided into two main parts. In the first part, silicone microemulsions were developed and characterized according to the Hydrophilic-Lipophilic Difference (HLD) framework. The hydrophobicity of silicone oils, the characteristic curvature of silicone surfactants and the co-surfactant contribution of methacrylic acid (MAA) and hydroxyethyl methacrylate (HEMA) were quantified. These findings led to the successful formulation of bicontinuous microemulsions (μEs) containing silicone oil, silicone alkyl polyether and reactive monomers in aqueous solution. Ternary phase diagrams of these systems revealed the potential for silicone-containing polymer composites with bicontinuous morphologies. In the second part of this study, the formulation and simultaneous polymerization of polydimethylsiloxane-poly(methacrylic acid – hydroxyethyl methacrylate), (PDMS-P(MAA-HEMA) IPNs from bicontinuous microemulsions was demonstrated. Laser scanning confocal microscopy (LSCM) on swollen polymers highlights aqueous pathways, and indicates the formation of bicontinuous morphologies with domain sizes at equilibrium swelling ranging from ~100 nm to 1 μm. Incorporating polymerizable surfactants into the microemulsion aided in stabilizing the initial microemulsion structure during polymerization. The process developed demonstrates a simple, single-step polymerization approach to forming IPNs from low viscosity microemulsion templates, and could potentially be extended to a variety of hydrophilic and hydrophobic monomers.

Interest in microemulsions as potential platforms for polymerization stems from the wide range of phase behaviour dependant morphologies and domain sizes that can be generated in a low viscosity environment. By introducing polymerizable components into the oil and aqueous phases of a microemulsion, we may essentially create a low viscosity, low interfacial tension, bicontinuous template with nanostructured morphologies and narrow domain size distributions analogous to those generated through conventional interpenetrating polymer network (IPN) synthesis and spinodal decomposition. The main objective of this dissertation is to test the application of bicontinuous microemulsion templates to the formulation and polymerization of a silicone-hydrogel IPN. In addition, the project expands on the classical definition of IPNs to a scale of entanglement at the level of groups of polymer chains, as opposed to molecular or chain-level entanglement. This study is divided into two main parts. In the first part, silicone microemulsions were developed and characterized according to the Hydrophilic-Lipophilic Difference (HLD) framework. The hydrophobicity of silicone oils, the characteristic curvature of silicone surfactants and the co-surfactant contribution of methacrylic acid (MAA) and hydroxyethyl methacrylate (HEMA) were quantified. These findings led to the successful formulation of bicontinuous microemulsions (μEs) containing silicone oil, silicone alkyl polyether and reactive monomers in aqueous solution. Ternary phase diagrams of these systems revealed the potential for silicone-containing polymer composites with bicontinuous morphologies. In the second part of this study, the formulation and simultaneous polymerization of polydimethylsiloxane-poly(methacrylic acid – hydroxyethyl methacrylate), (PDMS-P(MAA-HEMA) IPNs from bicontinuous microemulsions was demonstrated. Laser scanning confocal microscopy (LSCM) on swollen polymers highlights aqueous pathways, and indicates the formation of bicontinuous morphologies with domain sizes at equilibrium swelling ranging from ~100 nm to 1 μm. Incorporating polymerizable surfactants into the microemulsion aided in stabilizing the initial microemulsion structure during polymerization. The process developed demonstrates a simple, single-step polymerization approach to forming IPNs from low viscosity microemulsion templates, and could potentially be extended to a variety of hydrophilic and hydrophobic monomers.