Vitrimers
endow cross-linked polymers with malleability and reprocessability
via exchange reactions. However, designing of reprocessable, shape-memory
polymer materials with high strength via a catalyst-free method remains
a challenge under mild conditions. Here, we propose a facile strategy
to address this dilemma by introducing the exchangeable imine bond
and N-coordinated boroxine into a polybutadiene (PB)-based network.
Specifically, PB grafted with 2-aminoethanethiol is reacted with the
formyl group of phenylboronic acid and dehydrated to form a dual-dynamic
covalently cross-linked network at room temperature. The dynamic network
draws on the advantage of imine (toughness) and N-coordinated boroxine
(strength), making the PB-based materials exhibit favorable malleability,
mechanical property, reprocessability, and thermal-induced shape-memory
behavior. We can obtain customized high mechanical properties by tuning
the cross-linking density, and the tensile strength reaches a high
value (12.35 MPa) without fillers or any other additives. Meanwhile,
the unique network framework makes the material recycle over several
times without sacrificing its property. This work presents a facile
and effective approach to achieve a multifunctional polymer with customized
attributes. Besides, this strategy can recycle end-of-life rubber
to alleviate environmental pollution and provide inspiration for fabricating
targeted materials by uniting the dynamic covalent or noncovalent
bonds.