Catalyst-Free Self-Healing Bio-Based Polymers: Robust Mechanical Properties, Shape Memory, and Recyclability

The poor mechanical properties and disadvantages of catalysts limit the application of self-healing materials. To address these issues, catalyst-free self-healing bio-based polymers (AESO–EMPA polymers) with robust mechanical properties were prepared using epoxidized maleopimaric anhydride (EMPA) and aminated epoxidized soybean oil (AESO). The AESO–EMPA polymers are recyclable and exhibit self-healing and shape memory because of the dual-dynamic network of multiple H-bonds and dynamic ester bonds in the structure. Under the synergistic catalysis of the tertiary amines and hydroxyl groups originated from the polymers, the polymers in this study achieve network rearrangement without the need for additional catalysts. The polymers also exhibit excellent mechanical properties with a tensile strength of 29.1 ± 0.25 MPa and a Tg of 80.2 °C owing to the unique rigid backbone of rosin and the dual-dynamic network. The AESO–EMPA polymers can be used as reusable adhesives and exhibit excellent shear strength and repair rates.