Non-food biobased, isocyanate-free linear and network polyhydroxyuthane and polythiourethane: Recyclability with cross-link density recovery and excellent elevated-temperature creep resistance

While major efforts have been made to improve the renewability of linear and network non-isocyanate polyurethane (NIPU) and polythiourethane (NIPTU), no previous study has exploited non-food biobased precursors to synthesize NIPUs or NIPTUs. Here, we employ several non-food biobased monomers, including four cyclic carbonates, two cyclic thiocarbonates, and three amines, and employed different combinations of them to prepare a variety of NIPUs and NIPTUs with segmented linear or network structures. For segmented linear non-food biobased NIPUs, we demonstrate that different non-food biobased cyclic carbonates provide for excellent tunability of properties and behavior, e.g., noise damping, crystallizability, and nanophase separation. For network non-food biobased NIPU and NIPTU, we demonstrate their robustness and reprocessability, including full recovery of crosslink density after three melt-state recycling steps. In particular, NIPTU exhibit promising tensile performance and excellent high-temperature creep resistance, which has never before been reported.