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Nonisocyanate polyurethane (NIPU) is a research hotspot in polyurethane applications because it does not use phosgene. Herein, a novel method of solvent- and catalyst-free synthesis of a hybrid nonisocyanate polyurethane (HNIPU) is proposed. First, four diamines were used to react with ethylene carbonate to obtain four bis(hydroxyethyloxycarbonylamino)alkane (BHA). Then, BHA reacted with dimer acid under condensation in the melt to prepare four nonisocynate polyurethane prepolymers. Further, the HNIPUs were obtained by crosslinking prepolymers and resin epoxy and cured with the program temperature rise. In addition, four amines and two resin epoxies were employed to study the effects and regularity of HNIPUs. According to the results from thermal and dynamic mechanical analyses, those HNIPUs showed a high degree of thermal stability, and the highest 5% weight loss reached about 350 °C. More importantly, the utilization of these green raw materials accords with the concept of sustainable development. Further, the synthetic method and HNIPUs don’t need isocyanates, catalysts, or solvents.

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