Scaling Behavior and Structure–Property Relationships of Multifunctional Ternary-Hydrogels Based on N-Alkyl Methacrylate Esters: Property Tunability through Versatile Synthesis

Scaling behavior relating the synthesis conditions with swelling degree, preparation concentration and crosslinking density of multifunctional ternary-gels consisting of 2-(dimethylamino)ethyl methacrylate (DMAEMA), hydroxypropyl methacrylate (HPMA) and glycidyl methacrylate (GMA) is reported. Swelling is controlled by DMAEMA portion of terpolymers and DMAEMA-rich gels tended to swell more than GMA-rich gels and increase in GMA increase polymer-solvent interaction parameter, χ Critical conditions required for terpolymers to show phase transition are calculated as χ₁=0.4993 and χ₂=0.2959. Dependence of swelling degree ϕ_Von gel preparation concentration (Formula presented.) as a function of solvent quality is examined. Good solvent prediction of (Formula presented.) indicates a crossover between entanglement-dominated case and strongly cross-linked case corresponding to low and moderate degrees of swelling. Swelling of ternary-gels in different solvents shows that cyclohexanol is a good solvent and solubility parameter is 23.7 (MPa)^1/2. Addition of hydrophobic GMA leads to a significant increase in stiffness of terpolymer gels. Increase in elastic modulus as-prepared state is not monotonic and can be controlled by adjusting DMAEMA/GMA ratio since tertiary amine groups triggers cascading epoxy ring-opening reaction. Reduced modulus G_r decreased with increasing swelling degree and scaling relation between modulus and swelling is found as G_r ≈ (ϕ_V)^−0.66 which indicates that ternary-hydrogels, limited to weak stretching regime, obey Gaussian statistics.