Self-healing poly(oxime–carbamate) films with tunable mechanical properties derived from rosin

Thermoset polymers with superior dimensional stability and creep resistance have been widely used in various electronic and energy devices. However, they are difficult to reprocess and recycle, and with the gradual decrease in nonrenewable resources, there is an urgent need for new sustainable materials as alternatives to thermoset polymers. Polymer materials with self-healing properties can provide high durability and sustainability for devices. In this work, we prepared a series of rosin-based poly(oxime–carbamate) films by reacting rosin acrylate/glycidyl methacrylate ester with toluene 2, 4-diisocyanate using dimethylglyoxime as the chain extender and triethanolamine as the crosslinking agent. The introduction of rosin with a rigid tricyclic phenanthrene structure in the prepared films resulted in excellent tensile strength (4.9 ± 0.03 MPa) while maintaining high elongation at break (973.2 % ± 4.8 %) and toughness (20.9 ± 0.1 MJ m−3). The good self-healing properties of the prepared films (90.6 % ± 1.5 %, 60 °C for 3 h) were attributed to the introduction of dynamic oxime–carbamate bonds. In particular, the tunable mechanical and self-healing properties of the films can be achieved by varying the molar ratio of rosin acrylate/glycidyl methacrylate ester to dimethylglyoxime. Furthermore, the prepared rosin-based films exhibited good adhesion, welding, and anticorrosion properties. Considering the reversible exchange mechanism of dynamic oxime–carbamate bonds and their use in self-healing and recycling applications, a new strategy for developing sustainable high-performance biobased self-healing coatings is presented.