Design and application of functional polymers : from self-healing materials via hard tissue composites to methacrylate tougheners

The interdisciplinary interplay of macromolecular chemistry, organic chemistry and supramolecular chemistry within this thesis enabled the development of a range of functional polymers ranging from self-healing materials to hard scaffold (biocompatible) polymers and up to polymer particles as toughness modifiers. Attaching triazole-pyridine ligands into the side chain of a poly(lauryl methacrylate) based polymer and the subsequent complexation with appropriate iron(II) and cobalt(II) metal salts (FeCl2, FeBr2, Fe(OTf)2, CoCl2, CoBr2 and Co(BF4)2) enabled the fabrication of crosslinked metallocopolymer coatings with pronounced self-healing performances. The regioselective copper(I)-catalyzed 1,3-dipolar cycloaddition between multifunctional azides and terminal alkynes (CuAAC) represents the key step for the preparation of thermosets. Within the scope of this thesis the CuAAC was utilized to synthesize new polymeric materials with outstanding mechanical features under solvent-free conditions. Towards the biomedical application of 1,2,3-polytriazoles, the metal-free 1,3-dipolar cycloaddition of electron-poor alkynes and multifunctional azides was utilized for the fabrication of thermosets with interesting mechanical and biocompatible properties. Within the scope of this thesis core-shell particles consisting of an ethylene glycol dimethacrylate (EGDMA) crosslinked soft poly(butyl acrylate) (PBA) core and a hard Poly(methyl methacrylate) (PMMA) shell that was crosslinked in some cases with triethylene glycol dimethacrylate (TEGDMA). The incorporation of the lattices into a TEGDMA/ urethane dimethacrylate (UDMA) matrix and subsequently photo-polymerization of the monomer mixture caused an enhancement of fracture toughness and E-modulus of the resulting thermosets in comparison to the reference material.