Reprocessable polyhydroxyurethane networks exhibiting full property recovery and concurrent associative and dissociative dynamic chemistry via transcarbamoylation and reversible cyclic carbonate aminolysis

We discovered that polyhydroxyurethane (PHU) networks synthesized in the presence of a catalyst from five-membered cyclic carbonates are intrinsically reprocessable with full property recovery via transcarbamoylation exchange reactions and reversible cyclic carbonate aminolysis. Through a judicious choice of monomers, we demonstrated that PHU networks can be recycled multiple times with full property retention. The presence of reversible reactions in addition to exchange reactions in PHU network reprocessing should spur reconsideration of the underlying reprocessing chemistries associated with some dynamic covalent polymer networks which have been ascribed solely to exchange reactions. With excellent reprocessability, this synthetic framework also serves as a sustainable non-isocyanate-based alternative to traditional polyurethane (PU) networks.