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Hierarchically Structured Vitrimer Biocomposites for Sustainable Manufacturing.
Sargun Singh Rohewal1,2, Joshua T Damron2, Jiho Seo2
1Bredesen Center for Interdisciplinary Research and Graduate Education, University of Tennessee, Knoxville, TN, 37996, USA.
Small (Weinheim an Der Bergstrasse, Germany)
|June 18, 2025
Summary
This study introduces novel vitrimer composites with enhanced fiber-matrix bonding for sustainable manufacturing. These materials offer excellent mechanical properties and recyclability, overcoming key limitations in dynamic covalent polymer adoption.
Area of Science:
- Materials Science
- Polymer Chemistry
- Composite Materials
Background:
- Polymers with dynamic covalent bonds (DCBs) offer tunable properties, combining thermoplastic processability with thermoset performance.
- Challenges in determining the topology freezing temperature (Tv) and ensuring robust fiber-matrix adhesion hinder widespread adoption of DCB polymers.
- Vitrimers represent a class of DCB polymers with potential for sustainable manufacturing due to their recyclability.
Purpose of the Study:
- To develop and characterize novel epoxy-anhydride-based polyester vitrimer composites reinforced with cellulosic filaments.
- To investigate the role of dynamic interfacial bonding in enhancing composite performance and enabling thermal malleability.
- To elucidate the fundamental mechanisms governing vitrimeric transitions and their relationship to chemical bond exchange.
Main Methods:
- Fabrication of hierarchically structured vitrimer composites using cellulosic filaments.
- Assessment of mechanical properties, including shear strength and strain-to-failure.
- Utilisation of nuclear magnetic resonance (NMR) and nano-infrared (nano-IR) spectroscopies to study chemical bond dynamics.
- Evaluation of processability via vacuum-assisted resin transfer molding (VARTM).
- Testing of mechanical property retention after multiple thermal reforming cycles.
Main Results:
- Demonstrated exceptional mechanical properties with ≈70 MPa shear strength and >10% strain-to-failure.
- Established dynamic interfacial bonding through direct participation of cellulosic fiber hydroxyl groups in matrix transesterification.
- Provided spectroscopic evidence that chemical bond exchange initiates below the conventionally measured Tv.
- Showcased excellent processability using VARTM and high recyclability, retaining >90% of mechanical properties after multiple cycles.
- Supported the hypothesis that rheologically determined Tv is influenced by both chemical exchange and frictional dynamics.
Conclusions:
- Developed high-performance, sustainable vitrimer composites with enhanced interfacial adhesion and recyclability.
- Advanced the fundamental understanding of vitrimeric transitions, revealing a more complex transition mechanism than previously assumed.
- Highlighted the potential of these materials for sustainable manufacturing processes and advanced composite applications.
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