Advanced Manufacturing of Non-Isocyanate Polyurethanes by Chemical Design

Polyoxazolidones have shown promising applications as the result of their particular chemical reactivity. While promising, polyoxazolidones are relatively unexplored, especially in their manufacturing. This work focuses on finding new chemistries involving oxazolidones and combining them with advanced manufacturing, offering a platform for the development of this class of non-isocyanate polyurethanes. In Chapter 1, we describe state-of-the-art in 3D printing techniques and non isocyanate polyuirethanes. In Chapter 2, we implement extrusion-based 3D printing techniques together with dynamic materials with advanced properties. We develop phase separated materials with mechanical properties that are spatially tuned by selective thermal annealing. Chapter 3 is devoted to expanding the printability of these materials towards light-based 3D printing techniques. To do so, we develop a new photocuring procedure and systematically search for reactive diluents to have a desirable viscosity of the resin. In Chapter 4, we move to monomer design in order to endow the oxazolidone-based materials with degradability. We develop a new type of dynamic bond, study its formation and dynamics, and finally, introduce it in DLP printable materials with tuneable degradability. Chapter 5 describes further developments through monomer design where we heighten the hydrolytic stability of the network material at ambient conditions. We introduce a new dynamic bond in mechanically and chemically recyclable materials that are hydrolytically degradable. The last experimental chapter, Chapter 6, describes the implementation of dynamic oxazolidone crosslinkers in a proof-of-concept slippery coating for biomedical use. Finally, Chapter 7, holds the main conclusions from the experimental chapter together with a look at future developments of the materials here described.