High performance dynamic covalent crosslinked polyacylsemicarbazide composites with self-healing and recycling capabilities

Self-healing and recycling of fiber reinforced polymer (FRP) composites are of great significance towards pursuing a sustainable and circular economy, but remain a huge challenge due to the infusible and insoluble properties of thermoset polymers. The newly developed dynamic covalent polymers provide a great opportunity to resolve this issue for FRPs. Here we developed a novel type of dynamic covalently cross-linked polyacylsemicarbazide exhibiting a high modulus and self-healing/recycling capability due to the reversible properties of the dynamic acylsemicarbazide (ASC) moieties. Introducing different ASC moieties composed of different dihydrazides into the polymer can dramatically tune the mechanical, self-healing and reprocessing properties. An optimized polyacylsemicarbazide with a Young's modulus of ∼2.84 GPa, a stress at break of ∼100 MPa and a glass transition temperature of ∼123 °C exhibits a self-healing efficiency of ∼94.4% and great reprocessing properties. Furthermore, using this newly developed PASC material as the matrix resin, the carbon fiber reinforced polymer composite was successfully prepared through solution impregnation and thermal pressing. The composite exhibits an interlaminar shear strength of 40 MPa and a healing efficiency of 76.2%. The great dynamic reversible properties of ASC moieties enables the recycling of the carbon fiber and matrix resin, respectively, from the composites by a solvolysis method. Self-healing and recycling of fiber reinforced polymer (FRP) composites are of great significance towards pursuing a sustainable and circular economy, but remain a huge challenge due to the infusible and insoluble properties of thermoset polymers.