Natural processes continuously degrade a material’s performance throughout its life cycle. An emerging class of synthetic self-healing polymers and composites possess property-retaining functions with the promise of longer lifetimes. But sustained in-service repair of structural fiber-reinforced composites remains unfulfilled due to material heterogeneity and thermodynamic barriers in commonly cross-linked polymer-matrix constituents. Overcoming these inherent challenges for mechanical self-recovery is vital to extend in-service operation and attain widespread adoption of such bioinspired structural materials. Here we transcend existing obstacles and report a fiber-composite capable of minute-scale and prolonged in situ healing — 100 cycles: an order of magnitude higher than prior studies. By 3D printing a mendable thermoplastic onto woven glass/carbon fiber reinforcement and co-laminating with electrically resistive heater interlayers, we achieve in situ thermal remending of internal delamination via dynamic bond re-association. Full fracture recovery occurs below the glass-transition temperature of the thermoset epoxy-matrix composite, thus preserving stiffness during and after repair. A discovery of chemically driven improvement in thermal remending of glass- over carbon-fiber composites is also revealed. The marked lifetime extension offered by this self-healing strategy mitigates costly maintenance, facilitates repair of difficult-to-access structures (e.g., wind-turbine blades), and reduces part replacement, thereby benefiting economy and environment.
Recyclable high-performance epoxy based on transesterification reaction
Self-healing thermoset epoxy based on dynamic covalent bond chemistry has been developed in the past several years, which warrants the creation of recyclable epoxy. However, the existing systems produce epoxy that has lower strength, stiffness, and glass transition temperature, making them unsuitable for load-bearing structures. In this study, we developed a new recyclable thermoset epoxy through solid form recycling. The epoxy has strength, stiffness, and glass transition temperature similar to those found in conventional thermoset epoxy. The effect of healing temperature, healing time, healing pressure, and powder size on the healing efficiency was experimentally investigated. It was found that the healing efficiency is as high as 88.1%, and the epoxy can be recycled more than one time.
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- Award ID(s):
- 1736136
- NSF-PAR ID:
- 10072721
- Date Published:
- Journal Name:
- J. Mater. Chem. A
- Volume:
- 5
- Issue:
- 40
- ISSN:
- 2050-7488
- Page Range / eLocation ID:
- 21505 to 21513
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
null (Ed.)Self-healable and recyclable materials and electronics can improve the reliability and repairability and can reduce environmental pollution; therefore, they promise very broad applications. In this study, we investigated the self-healing performance of dynamic covalent thermoset polyimine and its nanocomposites based on the dynamic covalent chemistry. Heat press was applied to two laminating films of polyimine and its nanocomposites to induce self-healing. The effects of heat press time, temperature, and load on the interfacial shear strength of the rehealed films were investigated. The results showed that increasing the heat press time, temperature, and load can significantly improve the interfacial shear strength and thus the self-healing effect. For polyimine nanocomposites, increasing the heat press time, temperature, and load led to the improved electrical conductivity of the rehealed films.more » « less
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Dynamic bonds are a powerful approach to tailor the mechanical properties of elastomers and introduce shape-memory, self-healing, and recyclability. Among the library of dynamic crosslinks, electrostatic interactions among oppositely charged ions have been shown to enable tough and resilient elastomers and hydrogels. In this work, we investigate the mechanical properties of ionically crosslinked ethyl acrylate-based elastomers assembled from oppositely charged copolymers. Using both infrared and Raman spectroscopy, we confirm that ionic interactions are established among polymer chains. We find that the glass transition temperature of the complex is in between the two individual copolymers, while the complex demonstrates higher stiffness and more recovery, indicating that ionic bonds can strengthen and enhance recovery of these elastomers. We compare cycles to increasing strain levels at different strain rates, and hypothesize that at fast strain rates ionic bonds dynamically break and reform while entanglements do not have time to slip, and at slow strain rates ionic interactions are disrupted and these entanglements slip significantly. Further, we show that a higher ionic to neutral monomer ratio can increase the stiffness, but its effect on recovery is minimal. Finally, taking advantage of the versatility of acrylates, ethyl acrylate is replaced with the more hydrophilic 2-hydroxyethyl acrylate, and the latter is shown to exhibit better recovery and self-healing at a cost of stiffness and strength. The design principles uncovered for these easy-to-manufacture polyelectrolyte complex-inspired bulk materials can be broadly applied to tailor elastomer stiffness, strength, inelastic recovery, and self-healing for various applications.more » « less
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Carbon fiber reinforced polymer (CFRP) composites have been increasingly used to replace metal parts in many industries such as aerospace, marine, automotive, and sporting goods. The CFRP parts compared with their metallic counter parts have the advantages of lightweight, significantly higher tensile strength, stiffer, and corrosion resistant. On the other hand, compared with many metal parts, the CFRP parts have many well-known disadvantages including the lower toughness, lower through-thickness tensile and shear strengths, lower thermal conductivity, lower electrical conductivity, and lower operating temperature. These disadvantages have made the conversion from metal parts into CFRP parts challenging and costly to design, manufacture, and maintain. The use of nanoparticles in polymer has been studied in the recent two decades. Carbon nanotubes (CNTs) and carbon nanofibers (CNFs) have been dispersed in various thermoset and thermoplastic polymers and improved the mechanical, electrical, and thermal properties; however, the properties were not comparable to CFRP. Later, researchers tried to infuse CNTs or CNFs into either carbon fiber preforms [1] or glass fiber preforms [2] for improving the mechanical properties. But the results were marginal and with great uncertainty due to the challenges of nanoparticle dispersion, filtering, and alignment while being infused through the fiber preform. The glass fiber preform experiments ended with relatively more consistent improvement than the carbon fiber preform experiments since that the glass fiber preform has significantly larger pores than the carbon fiber preform' s. The small pore size presented a great challenge for infusing millions of unaligned long CNTs or CNFs through the carbon fiber preform without being filtered. To infuse long CNFs or CNTs through the carbon fiber preform and achieve reliable improvements, especially for 55% or higher carbon fiber volume fraction with increasingly tighter pores, an innovative plan for the processing and nano-reinforcing strategy is necessary. The z-threading strategy [3, 4, 5] has been reported to have consistent experimental successes in achieving the statistically meaningful improvement in multifunctional properties. The manufacturing steps of the CNF z-threaded CFRP (ZT-CFRP) are: (1) disperse the CNFs in a resin, (2) use a strong electrical field to align the CNFs in either the B-stage epoxy film or a CNF/resin impregnated sponge layer, whereas the CNFs are aligned in the through-thickness direction of the film or sponge layer. (3) place the resin film or sponge layer on a preheated dry carbon fiber fabric and press the resin film into the hot carbon fabric and allow the resin flow to carry the well-aligned CNFs to thread through the pores in the carbon fabric. (4) cool down the resin saturated and CNF z-threaded carbon fiber fabric to obtain the ZT-CFRP prepreg. (5) use the ZT-CFRP prepreg to make the ZT-CFRP laminate. Compared with the traditional CFRP, the ZT-CFRP laminates were reported of having improvement in the Mode-I delamination toughness, interlaminar shear strength, longitudinal compressive strength, through-thickness electrical conductivity, through-thickness thermal conductivity, and can reach the carbon fiber volume fraction of 55-80%. It is an effective approach to achieve a multifunctional CFRP for potentially expanding CFRP's applications.more » « less
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T g). POLYM. COMPOS., 40:2946–2953, 2019. © 2018 Society of Plastics Engineers
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/c7ta06397k
