Mechanically Interlocked Vitrimer Based on Polybenzoxazine and Polyrotaxane AITranslate

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DOI：https://doi.org/10.1021/acsapm.3c00196

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A mechanically interlocked vitrimer (MIV) based on a benzoxazine monomer and polyrotaxane (PR) has been prepared through a mechanically interlocked network (MIN) and dynamic covalent bond chemistry. The dynamic transacetalation exchange through the N,O-acetal-type polybenzoxazine (PBz) structure was catalyzed by a tin compound. Compared to the controlled PBz vitrimer without a MIN, the designed PBz MIV shows enhanced mechanical performance including ductility and tensile strength while maintaining relatively high Young’s modulus and glass transition temperature (Tg). The PBz MIV can be reprocessed several times without compromising mechanical performance and thermal stability. The PBz MIV also exhibits a faster dynamic bond exchange and a lower activation energy compared to the controlled PBz vitrimer due to the mobile intramolecular motions of PR in the network allowing for a dynamic bond exchange in the MIV more readily. The usefulness of the present study for the preparation of high-performance eco-friendly thermosetting vitrimers is discussed.