Dataset Information

Mechanically Robust, Recyclable, and Self-Healing Polyimine Networks.

ABSTRACT: To achieve energy saving and emission reduction goals, recyclable and healable thermoset materials are highly attractive. Polymer copolymerization has been proven to be a critical strategy for preparing high-performance polymeric materials. However, it remains a huge challenge to develop high-performance recyclable and healable thermoset materials. Here, polyimine dynamic networks based on two monomers with bulky pendant groups, which not only displayed mechanical properties higher than the strong and tough polymers, e.g., polycarbonate, but also excellent self-repairing capability and recyclability as thermosets are developed. Owing to the stability of conjugation effect by aromatic benzene rings, the final polyimine networks are far more stable than the reported counterparts, exhibiting excellent hydrolysis resistance under both alkaline condition and most organic solvents. These polyimine materials with conjugation structure can be completely depolymerized into monomers recovery in an acidic aqueous solution at ambient temperature. Resulting from the bulky pendant units, this method allows the exchange reactions of conjugation polyimine vitrimer easily within minutes for self-healing function. Moreover, the introduction of trifluoromethyl diphenoxybenzene backbones significantly increases tensile properties of polyimine materials. This work provides an effective strategy for fabricating high-performance polymer materials with multiple functions.

SUBMITTER: Yu P

PROVIDER: S-EPMC10323645 | biostudies-literature | 2023 Jul

REPOSITORIES: biostudies-literature

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Mechanically Robust, Recyclable, and Self-Healing Polyimine Networks.

Yu Ping P Wang Haiyue H Li Ting T Wang Guimei G Jia Zichen Z Dong Xinyu X Xu Yang Y Ma Qilin Q Zhang Dongen D Ding Hongliang H Yu Bin B

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20230423 19

To achieve energy saving and emission reduction goals, recyclable and healable thermoset materials are highly attractive. Polymer copolymerization has been proven to be a critical strategy for preparing high-performance polymeric materials. However, it remains a huge challenge to develop high-performance recyclable and healable thermoset materials. Here, polyimine dynamic networks based on two monomers with bulky pendant groups, which not only displayed mechanical properties higher than the stro ...[more]

PMID: 37088727

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Project description:Natural polymer hydrogels are one of the best biomaterials for soft tissue repair because of their excellent biocompatibility, biodegradability and low immune rejection. However, they lack mechanical strength matching that of natural tissue and desired functionality (e.g. self-healing and 3D-printability). To solve this problem, we developed a host-guest supramolecule (HGSM) with three arms covalently crosslinked with a natural polymer to construct a novel hydrogel with non-covalent bonds integrated in a covalently crosslinked network. The unique structure enabled the hydrogel to bear improved mechanical properties and show both self-healing and 3D printing capabilities. The three-armed HGSM was first prepared via the efficient non-covalent host-guest inclusion interactions between isocyanatoethyl acrylate-modified β-cyclodextrin (β-CD-AOI2) and acryloylated tetra-ethylene glycol-modified adamantane (A-TEG-Ad). Subsequently, a host-guest supramolecular hydrogel (HGGelMA) was obtained through copolymerization between the arms of HGSM and gelatin methacryloyl (GelMA) to form a covalently crosslinked network. The HGGelMA was robust, fatigue resistant, reproducible and rapidly self-healing. In HGGelMA, the covalent crosslinking maintained its overall shape whereas the weak reversible non-covalent host-guest interactions reinforced its mechanical properties and enabled it to rapidly self-heal upon fracturing. The reversible non-covalent interactions could be re-established upon breaking, so as to heal the hydrogel and dissipate energy to prevent catastrophic fracture propagation. Furthermore, the precursors of the HGGelMA were sufficiently viscous and could be rapidly photocrosslinked to produce a robust scaffold with an exquisite internal structure through 3D printing. The 3D-printed HGGelMA hydrogel scaffold was biocompatible, promoted cell adhesion and proliferation, and supported tissue in-growth. Our strategy of integrating non-covalently linked HGSM in a covalently linked hydrogel network represents a new approach to the development of natural polymers into biocompatible hydrogels with improved strength as well as desired self-healing and 3D-printability.

Dataset Information

Mechanically Robust, Recyclable, and Self-Healing Polyimine Networks.

Publications

Mechanically Robust, Recyclable, and Self-Healing Polyimine Networks.

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