Recyclable high-strength polybutadiene-based rubber with self-healing and shape memory properties via dynamic boronic ester and Diels-Alder chemistry

Dynamic cross-linked networks (DCNs) endow thermoset rubber with self-healability and recyclability to extend its lifetime and alleviate environmental pollution. However, the contradiction between high self-healing and mechanical properties in DCNs rubber is always difficult to be resolved. Herein, we used boronic ester (BO) and Diels-Alder dynamic covalent bonds (DA) to synthesize polybutadiene-based dual networks rubber (PB-BO-DA) via thiol-ene reaction. This approach achieved a tensile strength of 16.46 MPa and 99% self-healing efficiency, facilitated by extensive intermolecular interactions (π-π packing and N-B coordination) and fully dynamic cross-linking. In addition, multiple dynamic cross-linked networks (MDCNs) polybutadiene-based rubber also show excellent shape memory ability and recyclability. This strategy might open a helpful pathway to fabricate intelligent multifunctional polymers with high strength and high self-healing efficiency.