Robust Biobased Vitrimers and Its Application to Closed-Loop Recyclable Carbon Fiber-Reinforced Composites

Hong, Jiyae; Hong, Younggi; Jeong, Jisu; Oh, Dongki; Goh, Munju

doi:10.1021/acssuschemeng.3c03468

Cited by 12 publications

(8 citation statements)

References 61 publications

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“…The characteristic relaxation time (τ*) was measured by applying the test results to Maxwell’s model for viscoelastic fluids, as shown in eq G G normalo = exp ( − t τ ) where G , G o , t , and τ correspond to stress (MPa), initial stress (MPa), time (s), and relaxation time (s), respectively. The τ* is the time required for a material to reach 1/ e (37%) of its initial stress or modulus, where τ* decreases with increasing temperature . The τ* value for the ACO-DA-0.75 film was estimated to be 8095, 2130, 527, and 65 s for 100, 120, 140, and 160 °C, respectively.…”

Section: Resultsmentioning

confidence: 99%

Fully Biobased Self-Healing and Recyclable Covalent Adaptable Networks Prepared via a Catalyst-Free Aza-Michael Reaction

Kashyap,

Borah,

Shivam Shailesh Kumar

et al. 2024

ACS Appl. Polym. Mater.

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In the present scenario, petroleum resource-based thermoset materials have become an environmental threat due to their permanent cross-linked structure that limits their recyclability. To overcome this problem, the development of covalent adaptable networks (CANs) containing dynamic covalent bonds has emerged in recent years that can be recycled under suitable conditions. However, the development of fully biobased as well as recyclable CANs following a green synthetic protocol is yet a great challenge and a dream toward a sustainable environment. With this goal, here, we report the development of fully biobased CAN films from acrylated castor oil (a low-cost vegetable oil derivative) and cystamine (a biobased diamine) via a catalyst-free aza-Michael reaction using disulfide linkage as the dynamic covalent bond. The CAN films show excellent thermoself-healing behavior and recyclability for at least 10 cycles while maintaining their material properties. In addition, the CAN films can be catalytically degraded, which can be further reprocessed to reconstruct the films. Furthermore, the CAN films are hydrophobic in nature, indicating that these biobased recyclable CAN films are useful for protective surface coating applications. Therefore, as a proof of concept, we further demonstrate the anticorrosive properties of a film having a maximum water contact angle of 102.4°, analyzed by a polarization method, electrochemical impedance, and a salt spray fog test under a corrosive environment. This work provides an economical as well as environmentally friendly route to develop multifunctional materials for a sustainable future.

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Section: Resultsmentioning

confidence: 99%

Fully Biobased Self-Healing and Recyclable Covalent Adaptable Networks Prepared via a Catalyst-Free Aza-Michael Reaction

Kashyap,

Borah,

Shivam Shailesh Kumar

et al. 2024

ACS Appl. Polym. Mater.

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“…They are fabricated through lamination and molding methods. [40][41][42][43] For instance, epoxy resin-based CFRCs are fabricated through in situ thermal curing of a mixture containing CFs and epoxy prepolymers. [41] The sizing agents on the surface of CFs can bond with epoxy prepolymers to produce strong interfacial adhesion.…”

Section: Introductionmentioning

confidence: 99%

Upcycling of Carbon Fiber/Thermoset Composites into High‐Performance Elastomers and Repurposed Carbon Fibers

Yang,

Lu,

Wang

et al. 2024

Angewandte Chemie

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Recycling of carbon fiber‐reinforced polymer composites (CFRCs) based on thermosetting plastics is difficult. In the present study, high‐performance CFRCs are fabricated through complexation of aromatic pinacol‐cross‐linked polyurethane (PU‐AP) thermosets with carbon fiber (CF) cloths. PU‐AP thermosets exhibit a breaking strength of 95.5 MPa and toughness of 473.6 MJ m‐3 and contain abundant hydrogen‐bonding groups, which can have strong adhesion with CFs. Because of the high interfacial adhesion between CF cloths and PU‐AP thermosets and high toughness of PU‐AP thermosets, CF/PU‐AP composites possess a high tensile strength of >870 MPa. Upon heating in N,N‐dimethylacetamide (DMAc) at 100 °C, the aromatic pinacols in the CF/PU‐AP composites can be cleaved, generating non‐destructive CF cloths and linear polymers that can be converted to high‐performance elastomers. The elastomers are mechanically robust, healable, reprocessable, and damage‐resistant with an extremely high tensile strength of 74.2 MPa and fracture energy of 149.6 kJ m‐2. As a result, dissociation of CF/PU‐AP composites enables the recovery of reusable CF cloths and high‐performance elastomers, thus realizing the upcycling of CF/PU‐AP composites.

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“…Since their discovery, there have been proposed many pathways for designing vitrimers. 20,21 However, the migration and discompose of the catalysts used for vitrimer synthesis likely make the materials lose their reprocessability at last. In addition, some vitrimers, such as radical-mediated disulfide exchange type, may result a permanent covalent cross-linking and loss of reversible properties by the side reactions.…”

Section: Introductionmentioning

confidence: 99%

Room temperature‐responsive poly(vinyl hydroxyalkyl ether‐alt‐dialkyl maleate)‐based vitrimers with dynamic boronic ester bonds

Wang,

Xu,

Zhang

et al. 2024

J of Applied Polymer Sci

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Dynamic BO bonds are often applied to fabricate reversible‐cross‐linking and reprocessable polymer networks due to their high thermodynamic stability and kinetic tunability. However, it is still difficult to tailor boronic ester polymers, which have both excellent mechanical and self‐healing properties in the absence of external stimuli. To address the above challenge, a range of room‐temperature self‐healable vitrimers are prepared by the reactions of various poly(vinyl hydroxyalkyl ether‐alt‐dialkyl maleate) copolymers and 1,4‐phenyldiboronic acid. The dynamic cross‐linking networks offer the as‐prepared vitrimers superior mechanical properties and thermostability. Because of the presence of dynamic boronic ester bonds, the networks also demonstrated self‐healing (the tensile strength recovered to 83% after 3 days at room temperature) and reprocessing capabilities (no significant change in tensile strength after thrice process recycles). Moreover, the vitrimers have potential as promising damping materials with wide temperature windows around room temperature. For example, the vitrimer of poly(ethylene glycol monovinyl ether‐alt‐dibutyl maleate) and 1,4‐phenyldiboronic acid demonstrates its tanδmax 1.18, Tg = 6.2°C and effective damping temperature range is from −16.4 to 48.5°C.

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Robust Biobased Vitrimers and Its Application to Closed-Loop Recyclable Carbon Fiber-Reinforced Composites

Cited by 12 publications

References 61 publications

Fully Biobased Self-Healing and Recyclable Covalent Adaptable Networks Prepared via a Catalyst-Free Aza-Michael Reaction

Fully Biobased Self-Healing and Recyclable Covalent Adaptable Networks Prepared via a Catalyst-Free Aza-Michael Reaction

Upcycling of Carbon Fiber/Thermoset Composites into High‐Performance Elastomers and Repurposed Carbon Fibers

Room temperature‐responsive poly(vinyl hydroxyalkyl ether‐alt‐dialkyl maleate)‐based vitrimers with dynamic boronic ester bonds

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