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We demonstrate the functionalization of ABA triblock copolymer-based materials by introducing dynamic covalent bonded cross-links. The bond-exchange via trans-N-alkylation was operated in the domains of poly(4-vinylpyridine) end blocks, cross-linked by quaternization with dibromo cross-linkers, thus exhibiting vitrimer-like properties (e.g., softening and great stress relaxation) and other useful functions, such as re-processability, recyclability, and self-adhesion.

Graphical abstract: Functionalization of triblock copolymer elastomers by cross-linking the end blocks via trans-N-alkylation-based exchangeable bonds

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