Designing Multiphase Step-Growth Polymers for Advanced Technologies: From Electromechanical Transducers to Additive Manufacturing

The synthesis and characterization of step-growth polymers with novel monomers provided materials with tailored properties for emerging technologies. Specifically, multiphase materials (i.e., microphase separated block copolymers) exploit the synergistic relationship of combining polymers with disparate thermal and mechanical properties. The introduction of intramolecular interactions such as hydrogen and ionic bonding into these polymers further tailored their properties for applications including elastomers, electromechanical transducers, and additive manufacturing (AM). A review of recent literature revealed the material properties required for polymeric materials in electromechanical transducers, which aided in the design of polymers for this application.

An isocyanate-, catalyst-, and solvent-free approach facilitated the synthesis of segmented polyureas with tunable thermal and mechanical properties. These materials found use as high dielectric elastomers and water-soluble polymers for extrusion-based AM dependent on the backbone composition. Vat photopolymerization (VP) AM served as a technique to 3D printed novel unsaturated polyester resins (UPR). Incorporating a phosphonium ionic liquid as a reactive diluent replaced styrene and reduced the volatility of commonly used UPRs. VP successfully provided 3D structures from these UPRs that demonstrated limited ionic conductivities. An extensive review of the literature surrounding the structure-property relationships of charged block copolymers with varying architectures helped to inform the synthesis of novel, cationic step-growth polymers. The synthesis of a new phosphonium IL facilitated the synthesis of a segmented polyurethane containing a phosphonium-functionalized soft segment for the first time. This phosphonium polyurethane exhibited ionic conductivities comparable to literature examples of block copolymers used for ionic polymer transducers, which suggests that these materials may serve for this application as well. Carbonyldiimidazole provides a novel route towards synthesizing imidazolium ionenes with unique backbone structures. The coupling of poly(ethylene glycol) dibromides with a bis-carbonylimidazole monomer and a commercial aliphatic dibromide led to the formation of segmented imidazolium ionenes. These polymers exhibited significant atmospheric water uptake as well as water solubility. However, the physical properties of the materials suggested that the synthetic procedure resulted in low molecular weights. Suggested future work provides methods for circumventing this issue and proposes next steps for all the projects discussed herein.