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<p>Vitrimer systems, typically derived from complex and expensive thermosetting resins, are known for their dynamic covalent bonds that enable reprocessing, self-healing, and shape-memory capabilities. However, the intricate chemistry and processing involved in thermosetting systems limit their scalability and affordability for large-scale applications. In contrast, this study presents a novel and cost-effective approach by developing vitrimer systems based on thermoplastic copolymers, ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA) and ethylene-butyl acrylate-maleic anhydride (EBA-MAH), catalyzed by TBD (1,5,7-triazabicyclo[4.4.0]dec-5-ene). This method simplifies the chemistry involved in the vitrimer networks, making it easier and more economical to produce, with enhanced potential for scalable manufacturing. The aim of this study was to evaluate the impact of TBD concentration on the mechanical properties, shape-memory performance, and activation energy of these materials. The results indicate that increasing the TBD concentration improves the crosslinking density, enhancing shape-memory performance. The recovery rate increased from 86.66 for the 0% TBD system to 99.90% for the 5% TBD system, while the shape fixation improved from 62.00 to 80.00%. Additionally, the activation energy for stress relaxation decreased with increasing TBD concentration, with values of 85.9&#xa0;kJ/mol, 79.6&#xa0;kJ/mol, and 75.0&#xa0;kJ/mol for 1%, 3%, and 5% TBD, respectively. This decrease in activation energy suggests that higher TBD concentrations facilitate faster bond exchange reactions, improving reprocessability. The materials also exhibited increased rigidity with higher TBD concentrations, with a corresponding increase in the storage modulus, while maintaining flexibility due to the rubber nature of the copolymers. These findings demonstrate the potential of TBD-catalyzed vitrimer systems as scalable and cost-effective solutions for reprocessable materials with dynamic properties, offering a simple alternative to traditional thermosetting systems.</p> Graphical Abstract <p></p>

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Scaling up vitrimers: developing thermoplastic-based dynamic networks via epoxy–anhydride reactions

  • 期刊论文

  • 发表日期：

    2025年9月2日

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  • Rafael Braga da Cunha,
  • Marcela Cristine de Alencar Lira,
  • Válmer Azevedo de Sousa Filho,
  • Alexandre da Silva Lúcio,
  • Pankaj Agrawal,
  • Gustavo de Figueiredo Brito,
  • Tomás Jeferson Alves de Mélo

摘要

Vitrimer systems, typically derived from complex and expensive thermosetting resins, are known for their dynamic covalent bonds that enable reprocessing, self-healing, and shape-memory capabilities. However, the intricate chemistry and processing involved in thermosetting systems limit their scalability and affordability for large-scale applications. In contrast, this study presents a novel and cost-effective approach by developing vitrimer systems based on thermoplastic copolymers, ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA) and ethylene-butyl acrylate-maleic anhydride (EBA-MAH), catalyzed by TBD (1,5,7-triazabicyclo[4.4.0]dec-5-ene). This method simplifies the chemistry involved in the vitrimer networks, making it easier and more economical to produce, with enhanced potential for scalable manufacturing. The aim of this study was to evaluate the impact of TBD concentration on the mechanical properties, shape-memory performance, and activation energy of these materials. The results indicate that increasing the TBD concentration improves the crosslinking density, enhancing shape-memory performance. The recovery rate increased from 86.66 for the 0% TBD system to 99.90% for the 5% TBD system, while the shape fixation improved from 62.00 to 80.00%. Additionally, the activation energy for stress relaxation decreased with increasing TBD concentration, with values of 85.9 kJ/mol, 79.6 kJ/mol, and 75.0 kJ/mol for 1%, 3%, and 5% TBD, respectively. This decrease in activation energy suggests that higher TBD concentrations facilitate faster bond exchange reactions, improving reprocessability. The materials also exhibited increased rigidity with higher TBD concentrations, with a corresponding increase in the storage modulus, while maintaining flexibility due to the rubber nature of the copolymers. These findings demonstrate the potential of TBD-catalyzed vitrimer systems as scalable and cost-effective solutions for reprocessable materials with dynamic properties, offering a simple alternative to traditional thermosetting systems.

Graphical Abstract