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Recyclable Polyester Thermosets and Reinforced Composites

Category: Mechanical/Materials
Developers: Oak Ridge National Laboratory


Product Description:This work demonstrates the fabrication of tough, hierarchically structured epoxy–anhydride vitrimer composites reinforced with cellulosic, glass or surface-tailored carbon fibers. These composites show remarkable strength, ductility, and malleability. The chemical bond exchange initiates at temperatures well below the rheologically determined vitrification temperature, suggesting that traditional thermosets can now be recycled. Polymers that incorporate dynamic covalent bonds exhibit thermoplastic-like flow above their vitrification temperature (Tv) while retaining thermoset-like properties below it, making them promising for sustainable manufacturing. This technology harnesses the dynamic nature of covalently adaptive networks to develop tough VCs reinforced with cellulosic filaments. By precisely tuning the epoxy–anhydride matrix composition and strategically leveraging dynamic covalent interactions at the fiber–matrix interface, it achieves exceptional mechanical performance, including high strength (~130 MPa), significant ductility (>10% strain-to-failure) and malleability upon thermal activation. The bulk reinforced composite exhibits excellent creep resistance, exceptional toughness caused by interfacial bonding, and thermoset-like performance below 120°C, yet can be remolded between 150°C‒180°C. These fundamental insights, coupled with our scalable fabrication strategy compatible with industrial processes such as VARTM, position these VCs as promising candidates for next-generation sustainable materials, offering not only exceptional mechanical performance but also closed-loop recyclability.


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