High performance, self-healable and recyclable epoxy thermosets by integrating dynamic hindered urea bonds

During recent decades, intrinsic self-healable thermosetting materials by integrating dynamic covalent bonds (DCBs) have been widely used. In this study, through the molecular structure design, a flexible polyurethane curing agent based on hindered urea bonds (HUBs) was successfully prepared by the reaction of Hexamethylene diisocyanate trimer (THDI) and sterically hindered secondary amine, which was further used as a curing agent to cure epoxy resin. Therefore, a new type of epoxy thermosetting material (TBEP) with dynamic hindered urea bond was synthesized and the preparation and performance of TBEP were confirmed and characterized by infrared spectroscopy, thermomechanical analysis and thermal stability test. The results show that the HUBs are successfully integrated into the epoxy resin and endow the epoxy thermosets with brilliant self-healable, reprocessable, recyclable and shape memory properties. Simultaneously, the existence of flexible polyurethane chain in the crosslinking network effectively solves the brittleness problem of epoxy resin, promotes the mechanical performance of epoxy thermosets, and further broadens the its application field. This work provides a simple and efficient method to design flexible and self-healable epoxy thermosets with brilliant mechanical performance, which solves the contradiction between outstanding mechanical properties and self-healing ability of epoxy resin to some extent, and is environmentally friendly and cost-effective in acquisition and application.