Healable and Recyclable Elastomers with Record‐High Mechanical Robustness, Unprecedented Crack Tolerance, and Superhigh Elastic Restorability

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(27)

Published: June 1, 2021

Abstract Spider silk is one of the most robust natural materials, which has extremely high strength in combination with great toughness and good elasticity. Inspired by spider but beyond it, a healable recyclable supramolecular elastomer, possessing superhigh true stress at break (1.21 GPa) ultrahigh (390.2 MJ m −3 ), are, respectively, comparable to ≈2.4 times higher than those typical silk, developed. The elastomer highest tensile (ultimate engineering stress, 75.6 MPa) ever recorded for polymeric elastomers, rendering it strongest toughest thus far. hyper‐robust exhibits superb crack tolerance unprecedentedly fracture energy (215.2 kJ −2 ) that even exceeds metals alloys, elastic restorability allowing dimensional recovery from elongation over 12 times. These extraordinary mechanical performances mainly originate meticulously engineered hydrogen‐bonding segments, consisting multiple acylsemicarbazide urethane moieties linked flexible alicyclic hexatomic spacers. Such incorporated between extensible polymer chains, aggregate form geometrically confined hydrogen‐bond arrays resembling silk. act as firm reversible crosslinks sacrificial bonds enormous dissipation, conferring exceptional robustness, healability, recyclability on elastomer.

Language: Английский

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Healable, Recyclable, and Mechanically Tough Polyurethane Elastomers with Exceptional Damage Tolerance

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(50)

Published: Nov. 11, 2020

Abstract There is a huge requirement of elastomers for use in tires, seals, and shock absorbers every year worldwide. In view sustainable society, the next generation expected to combine outstanding healing, recycling, damage‐tolerant capacities with high strength, elasticity, toughness. However, it remains challenging fabricate such because mechanisms properties mentioned above are mutually exclusive. Herein, fabrication healable, recyclable, mechanically tough polyurethane (PU) damage tolerance by coordination multiblock polymers poly(dimethylsiloxane) (PDMS)/polycaprolactone (PCL) containing hydrogen bonding motifs Zn 2+ ions reported. The organization bipyridine groups coordinated ions, carbamate cross‐linked bonds, crystallized PCL segments generates phase‐separated dynamic hierarchical domains. Serving as rigid nanofillers capable deformation disintegration under an external force, domains can strengthen significantly enhance their toughness fracture energy. As result, exhibit tensile strength ≈52.4 MPa, ≈363.8 MJ m −3 , exceptional energy ≈192.9 kJ −2 . Furthermore, be conveniently healed recycled regain original mechanical integrity heating.

Language: Английский

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Material properties and applications of mechanically interlocked polymers

Nature Reviews Materials, Journal Year: 2021, Volume and Issue: 6(6), P. 508 - 530

Published: Feb. 12, 2021

Language: Английский

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Extremely Strong and Tough Biodegradable Poly(urethane) Elastomers with Unprecedented Crack Tolerance via Hierarchical Hydrogen‐Bonding Interactions

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(21)

Published: Feb. 23, 2023

The elastomers with the combination of high strength and toughness have always been intensively pursued due to their diverse applications. Biomedical applications frequently require biodegradability biocompatibility properties. It remains a great challenge prepare biodegradable extremely robust mechanical properties for in vivo use. In this report, we present polyurethane elastomer unprecedented application as hernia patches, which was obtained by solvent-free reaction polycaprolactone (PCL) isophorone diisocyanate (IPDI) N,N-bis(2-hydroxyethyl)oxamide (BHO) chain extender. Abundant hierarchical hydrogen-bonding interactions inside hinder crystallization PCL segments facilitate formation uniformly distributed hard phase microdomains, miraculously realize fracture 92.2 MPa true stress 1.9 GPa, while maintaining elongation-at-break ≈1900% ultrahigh 480.2 MJ m-3 energy 322.2 kJ m-2 . Hernia patches made from via 3D printing technology exhibit outstanding properties, biocompatibility, biodegradability. demonstrate considerable potentials

Language: Английский

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Molecular engineering of a colorless, extremely tough, superiorly self-recoverable, and healable poly(urethane–urea) elastomer for impact-resistant applications

Materials Horizons, Journal Year: 2021, Volume and Issue: 8(8), P. 2238 - 2250

Published: Jan. 1, 2021

Molecular engineering of a microphase separated structure to convert weak, soft and self-healing polymer strong, tough, resilient, healable poly(urethane–urea) elastomer, which is in great demand for transparent protection engineering.

Language: Английский

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Highly compressible glass-like supramolecular polymer networks

Nature Materials, Journal Year: 2021, Volume and Issue: 21(1), P. 103 - 109

Published: Nov. 25, 2021

Language: Английский

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Room-temperature self-healing supramolecular polyurethanes based on the synergistic strengthening of biomimetic hierarchical hydrogen-bonding interactions and coordination bonds

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 451, P. 138673 - 138673

Published: Aug. 18, 2022

Language: Английский

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Mechanically Interlocked Vitrimers

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 144(2), P. 872 - 882

Published: Dec. 21, 2021

Mechanically interlocked networks (MINs) have emerged as an encouraging platform for the development of mechanically robust yet adaptive materials. However, difficulty in reversibly breaking mechanical bonds poses a real challenge to MINs customizable and sustainable Herein, we couple vitrimer chemistry with structures generate new class MINs─referred vitrimers (MIVs)─to address challenge. Specifically, prepared acetoacetate-decorated [2]rotaxane that undergoes catalyst-free condensation reaction two commercially available multiamine monomers furnish MIVs. Compared control whose wheels are nonslidable under applied force, our MIVs slidable motifs showcase enhanced performance including Young's modulus (18.5 ± 0.9 vs 1.0 0.1 MPa), toughness (3.7 MJ/m3), damping capacity (98% 72%). The structural basis behind unique property profiles is demonstrated be force-induced host-guest dissociation consequential intramolecular sliding along axles. peculiar behaviors represent consecutive energy dissipation mechanism, which provides complement other pathways mainly depend on sacrificial bonds. Moreover, by virtue vinylogous urethanes, impart reprocessability chemical recyclability MINs, thereby empowering reconfiguration without Finally, it disclosed motions [2]rotaxanes could accelerate dynamic exchange urethane via loosening network, suggestive synergistic effect between dual entities.

Language: Английский

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Engineering of Chain Rigidity and Hydrogen Bond Cross‐Linking toward Ultra‐Strong, Healable, Recyclable, and Water‐Resistant Elastomers

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(21)

Published: Feb. 28, 2023

High-performance elastomers have gained significant interest because of their wide applications in industry and our daily life. However, it remains a great challenge to fabricate simultaneously integrating ultra-high mechanical strength, toughness, excellent healing recycling capacities. In this study, ultra-strong, healable, recyclable are fabricated by dynamically cross-linking copolymers composed rigid polyimide (PI) segments soft poly(urea-urethane) (PUU) with hydrogen bonds. The elastomers, which denoted as PIPUU, record-high tensile strength ≈142 MPa an extremely high toughness ≈527 MJ m-3 . structure the PIPUU elastomer contains hydrogen-bond-cross-linked elastic matrix homogenously dispersed nanostructures. PI self-assemble generate phase-separated nanostructures that serve nanofillers significantly strengthen elastomers. Meanwhile, is PUU cross-linked reversible bonds, largely enhance elastomer. can be healed recycled restore original strength. Moreover, performance hydrophobic segments, scratch-, puncture-, water-resistant.

Language: Английский

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Mechanically interlocked polymers based on rotaxanes

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(16), P. 7046 - 7065

Published: Jan. 1, 2022

The nature of mechanically interlocked molecules (MIMs) has continued to encourage researchers design and construct a variety high-performance materials. Introducing structures into polymers led novel polymeric materials, called (MIPs). Rotaxane-based MIPs are an important class, where the characteristic retains high degree structural freedom mobility their components, such as rotation sliding motions rotaxane units. Therefore, these MIP materials known possess unique set properties, including mechanical robustness, adaptability responsiveness, which endow them with potential applications in many emerging fields, protective intelligent actuators, mechanisorption. In this review, we outline synthetic strategies, structure-property relationships, application explorations various polyrotaxanes, linear polyrotaxane networks, dendrimers.

Language: Английский

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