Preparation of Styrene–Butadiene Rubber Vitrimers with High Strength and Toughness through Imine and Hydrogen Bonds

The covalent cross-linked structure imparts strong elasticity and environmental resistance to elastomers, while the irreversibility of covalent bonds restricts the recycling of rubbers. Integrating vitrimer chemistry into chemical cross-linked networks appears to be a charming method to combine the exciting properties of thermoplastics and thermosets. However, it is still a challenge to design a rubber vitrimer with robust mechanical properties. Here, inspired by supramolecular interactions associated with natural materials, we demonstrated a dual reversible cross-linked SBR vitrimer by introducing imine bonds and hydrogen bonding. The integration of hydrogen bonding endows the elastomer vitrimer with significantly improved strength and toughness without influencing the recycling ability. This work provides a simple and effective strategy in the design of elastomer vitrimers with robust mechanical properties and good recyclability.