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<p>Bio-based vitrimers represent a promising route toward sustainable polymer networks that combine recyclability, repairability, and functional performance. In this work, a fully bio-based and catalyst-free vitrimer was developed from epoxidized linseed oil (ELO) and tartaric acid (TA), aiming to integrate vitrimer behavior with shape-memory and self-healing functionalities at moderate activation temperatures. The materials were prepared by curing ELO with TA at different epoxy: acid molar ratios, forming dynamic ester networks through epoxy–acid reactions. The systems were characterized by FTIR, DMA, swelling and gel content, rheology, stress relaxation, mechanical testing, shape-memory cycles, self-healing, and reprocessing experiments. Spectroscopic analysis confirmed epoxy consumption and ester formation. Increasing the epoxy: acid ratio increased gel content (83.3–93.5%), stiffness, and tensile strength, while reducing swelling, elongation at break, and impact strength. All compositions exhibited a glass transition near 50&#xa0;°C. Stress-relaxation experiments revealed vitrimer behavior, with rapid relaxation above Tg and activation energies between 49 and 71&#xa0;kJ·mol⁻¹. Excellent shape-memory performance was achieved, with shape fixity of ~ 90% and shape recovery between 95 and 97%. The materials also showed efficient self-healing and reprocessing, with visual crack closure and recovery of more than 90% of mechanical properties after reprocess. These results demonstrate that epoxidized linseed oil and tartaric acid form an efficient, sustainable vitrimer platform combining recyclability, self-healing, and shape-memory behavior, with potential applications in smart materials, recyclable, and self-repairing polymer systems.</p> Graphical Abstract <p></p>

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Fully Biobased Catalyst-Free Vitrimer from Epoxidized Linseed Oil and Tartaric Acid Exhibiting Shape-Memory and Self-Healing Properties

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月29日

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  • Jociele Cristine Alves Nogueira,
  • Fabricio Ravell Silva Sousa,
  • Rafael Braga da Cunha,
  • Marcela Cristine de Alencar Lira,
  • Jaini Miscilene de Araújo,
  • Válmer Azevedo de Sousa Filho,
  • Ryan Lucas Pereira Bonfim,
  • Pankaj Agrawal,
  • Tomás Jeferson Alves de Mélo,
  • Gustavo de Figueiredo Brito

摘要

Bio-based vitrimers represent a promising route toward sustainable polymer networks that combine recyclability, repairability, and functional performance. In this work, a fully bio-based and catalyst-free vitrimer was developed from epoxidized linseed oil (ELO) and tartaric acid (TA), aiming to integrate vitrimer behavior with shape-memory and self-healing functionalities at moderate activation temperatures. The materials were prepared by curing ELO with TA at different epoxy: acid molar ratios, forming dynamic ester networks through epoxy–acid reactions. The systems were characterized by FTIR, DMA, swelling and gel content, rheology, stress relaxation, mechanical testing, shape-memory cycles, self-healing, and reprocessing experiments. Spectroscopic analysis confirmed epoxy consumption and ester formation. Increasing the epoxy: acid ratio increased gel content (83.3–93.5%), stiffness, and tensile strength, while reducing swelling, elongation at break, and impact strength. All compositions exhibited a glass transition near 50 °C. Stress-relaxation experiments revealed vitrimer behavior, with rapid relaxation above Tg and activation energies between 49 and 71 kJ·mol⁻¹. Excellent shape-memory performance was achieved, with shape fixity of ~ 90% and shape recovery between 95 and 97%. The materials also showed efficient self-healing and reprocessing, with visual crack closure and recovery of more than 90% of mechanical properties after reprocess. These results demonstrate that epoxidized linseed oil and tartaric acid form an efficient, sustainable vitrimer platform combining recyclability, self-healing, and shape-memory behavior, with potential applications in smart materials, recyclable, and self-repairing polymer systems.

Graphical Abstract