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Supramolecularly engineered benzoxazine networks for intrinsic self-healing and shape memory applications.

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Title: Supramolecularly engineered benzoxazine networks for intrinsic self-healing and shape memory applications.
Authors: Revathi, A.1,2 (AUTHOR), Krishnadevi, K.3 (AUTHOR) krishchem05@gmail.com, Prasanna, D.4 (AUTHOR), Bharath, P.1 (AUTHOR), Ramachandhran, D.1 (AUTHOR) ittakavirc@gmail.com
Source: Journal of Polymer Research. Jun2026, Vol. 33 Issue 6, p1-14. 14p.
Subjects: Self-healing materials, Shape memory polymers, Polyurethanes, Thermal stability, Supramolecular chemistry, Antimicrobial polymers, Benzoxazines, Hydrogen bonding
Abstract: Bio-based poly(urethane-benzoxazine) networks exhibiting temperature assisted autonomous self-healing were engineered through reversible supramolecular hydrogen bonding interactions. A renewable benzoxazine precursor was synthesized via a Mannich condensation of eugenol, JEFFAMINE T-403, and paraformaldehyde, and subsequently co-polymerized with 2-mercaptoethanol and controlled loadings of hexamethylene diisocyanate to generate hybrid thiol incorporated benzoxazine with polyurethane architectures. Structural elucidation of the monomer and polymer networks was confirmed by 1H NMR and FT-IR spectroscopy. Thermal stability of the material was investigated using TGA and DSC, revealing tuneable thermal behaviour as a function of polyurethane content. The maximum degradation temperature of EJ polymer is 376 °C and the Tg values of polymer composites like P(EJ-n), P(EJ-SH), P(EJ-SH-co-PU1) and P(EJ-SH-co-PU2) is 238 °C, 241 °C, 268 °C, and 270 °C respectively. Self-healing performance was quantified using tensile testing and Shore-D hardness recovery across multiple healing cycles and the self-healing efficiency is up to 83%, and was supported by morphological assessment via SEM and optical microscopy. Contact angle measurements demonstrated increasing hydrophilicity with higher polyurethane incorporation, correlating with enhanced polymer chain mobility and dynamic supramolecular interactions responsible for efficient network reconfiguration and the contact angle reduction of EJ polymer composites is 100º to 88º. The cyclic shape-memory performance of P(EJ-SH-co-PU2) polymer is quantitatively calculated with shape fixity ratio (Rf) and shape recovery ratio (Rr) and it gives Rf ratio is > 93% and Rr ratio is > 92%. The materials displayed robust self-healing efficiency, thermomechanical stability, and noticeable shape memory behaviour arising from reversible urethane with thiol/benzoxazine hydrogen bonding moieties. Additionally, the hybrid polymers exhibited notable antimicrobial activity, underscoring their potential for high performance, multifunctional, and sustainable smart material applications. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
Description
Abstract:Bio-based poly(urethane-benzoxazine) networks exhibiting temperature assisted autonomous self-healing were engineered through reversible supramolecular hydrogen bonding interactions. A renewable benzoxazine precursor was synthesized via a Mannich condensation of eugenol, JEFFAMINE T-403, and paraformaldehyde, and subsequently co-polymerized with 2-mercaptoethanol and controlled loadings of hexamethylene diisocyanate to generate hybrid thiol incorporated benzoxazine with polyurethane architectures. Structural elucidation of the monomer and polymer networks was confirmed by 1H NMR and FT-IR spectroscopy. Thermal stability of the material was investigated using TGA and DSC, revealing tuneable thermal behaviour as a function of polyurethane content. The maximum degradation temperature of EJ polymer is 376 °C and the Tg values of polymer composites like P(EJ-n), P(EJ-SH), P(EJ-SH-co-PU1) and P(EJ-SH-co-PU2) is 238 °C, 241 °C, 268 °C, and 270 °C respectively. Self-healing performance was quantified using tensile testing and Shore-D hardness recovery across multiple healing cycles and the self-healing efficiency is up to 83%, and was supported by morphological assessment via SEM and optical microscopy. Contact angle measurements demonstrated increasing hydrophilicity with higher polyurethane incorporation, correlating with enhanced polymer chain mobility and dynamic supramolecular interactions responsible for efficient network reconfiguration and the contact angle reduction of EJ polymer composites is 100º to 88º. The cyclic shape-memory performance of P(EJ-SH-co-PU2) polymer is quantitatively calculated with shape fixity ratio (Rf) and shape recovery ratio (Rr) and it gives Rf ratio is > 93% and Rr ratio is > 92%. The materials displayed robust self-healing efficiency, thermomechanical stability, and noticeable shape memory behaviour arising from reversible urethane with thiol/benzoxazine hydrogen bonding moieties. Additionally, the hybrid polymers exhibited notable antimicrobial activity, underscoring their potential for high performance, multifunctional, and sustainable smart material applications. [ABSTRACT FROM AUTHOR]
ISSN:10229760
DOI:10.1007/s10965-026-04973-9