Reinforced, self-healing, recyclable rubber materials based on multiple dynamic bond constructs crosslinked with chemical groups

Enhancing the mechanical attributes of traditional rubber, while simultaneously imparting superior self-healing and recyclability, remains a formidable task within the realm of polymer science. In this study, we introduce, for the inaugural time, the utilization of metal–ligand interactions to amalgamate chemical cross-linking sites within a styrene-butadiene rubber matrix. This approach facilitates the creation of a fortified, self-healing, and recyclable rubber composite, interconnected by an array of dynamic bonds within a singular chemical entity. This chemical assembly engenders a microphase-separated architecture that exhibits reinforcement and resistance to creep. In addition, the presence of reversible oxime-carbamate and metal–ligand bonds bestow the rubber composites with remarkable self-healing and recyclability. Notably, the self-healing efficiency reached an impressive 87%, while the recyclability retention hovered between 85 and 91% (in terms of tensile strength) post multiple reprocesses. This research paves a novel avenue for the fabrication of rubber composites that are robust, self-healing, and recyclable.