High‐Performance Polymeric Materials through Hydrogen‐Bond Cross‐Linking

Advanced Materials, Journal Year: 2019, Volume and Issue: 32(18)

Published: June 19, 2019

Abstract It has always been critical to develop high‐performance polymeric materials with exceptional mechanical strength and toughness, thermal stability, even healable properties for meeting performance requirements in industry. Conventional chemical cross‐linking leads enhanced thermostability at the expense of extensibility due mutually exclusive mechanisms. Such major challenges have recently addressed by using noncovalent reversible multiple hydrogen‐bonds (H‐bonds) that widely exist biological materials, such as silk muscle. Recent decades witnessed development many tailor‐made H‐bond cross‐linked materials. Here, recent advances strategies are reviewed creating polymers can be realized via i) self‐association interchain H‐bonding interactions or specific motifs, 2‐ureido‐4‐pyrimidone units self‐complementary quadruple H‐bonds ii) addition external cross‐linkers, including small molecules, nanoparticles, polymer aggregates. The resultant normally exhibit tunable high strength, large extensibility, improved thermostability, capability. portfolios enable these advanced find significant cutting‐edge applications. Major facing existing discussed, some promising approaches designing future also proposed.

Language: Английский

---

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

---

Mechanically Robust, Elastic, and Healable Ionogels for Highly Sensitive Ultra‐Durable Ionic Skins

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

Published: June 26, 2020

The fabrication of highly durable skin-mimicking sensors remains challenging because the unavoidable fatigue and physical damage that are subjected to in practical applications. In this study, ultra-durable ionic skins (I-skins) with excellent healability high sensitivity fabricated by impregnating liquids (ILs) into a mechanically robust poly(urea-urethane) (PU) network. PU network is composed crystallized poly(ε-caprolactone) flexible poly(ethylene glycol) dynamically cross-linked hindered urea bonds hydrogen bonds. Such design endows resultant ionogels mechanical strength, good elasticity, Young's modulus similar natural skin, healability. ionogel-based I-skins exhibit wide range strains (0.1-300%) pressures (0.1-20 kPa). Importantly, show reproducible electrical response over 10 000 uninterrupted strain cycles. sensing performance stored open air for 200 days almost same as freshly prepared I-skin. fractured can be easily healed heating at 65 °C restores their original performance. long-term durability attributed combination non-volatility ILs, healability, well-designed properties.

Language: Английский

---

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

---

Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors

Nature Communications, Journal Year: 2019, Volume and Issue: 10(1)

Published: Nov. 26, 2019

The emergence of wearable electronics puts batteries closer to the human skin, exacerbating need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy overcome canonical tradeoff between mechanical robustness ionic conductivity in polymer electrolytes. lithium ion conductor utilizes orthogonally functional H-bonding domains ion-conducting create electrolyte with unprecedented toughness (29.3 MJ m-3) high (1.2 × 10-4 S cm-1 at 25 °C). Implementation binder material allows creation stretchable lithium-ion electrodes strain capability over 900% via conventional slurry process. nature these components enables intimate bonding electrode-electrolyte interface. Combination leads capacity 1.1 mAh cm-2 functions even when stretched 70% strain. method reported here decoupling from properties opens promising route high-toughness transport energy storage applications.

Language: Английский

---

Natural skin-inspired versatile cellulose biomimetic hydrogels

Journal of Materials Chemistry A, Journal Year: 2019, Volume and Issue: 7(46), P. 26442 - 26455

Published: Jan. 1, 2019

A skin-like cellulose biomimetic hydrogel was prepared based on dynamic covalent chemistry, which realized the combination of ultra-stretchability, self-healing, adhesiveness, antibacterial and mechano-stimuli sensitivity within a single structure.

Language: Английский

---

Extrusion 3D Printing of Polymeric Materials with Advanced Properties

Advanced Science, Journal Year: 2020, Volume and Issue: 7(17)

Published: Aug. 5, 2020

Abstract 3D printing is a rapidly growing technology that has an enormous potential to impact wide range of industries such as engineering, art, education, medicine, and aerospace. The flexibility in design provided by this technique offers many opportunities for manufacturing sophisticated devices. most widely utilized method extrusion‐based solid‐freeform fabrication approach, which extremely attractive additive both academic industrial research communities. This versatile, with the ability print dimensions, multimaterial, multifunctional structures. It also very affordable prototyping. However, lack variety printable polymers advanced material properties becomes main bottleneck further development technology. Herein, comprehensive review provided, focusing on strategies achieve or enhance printability including thermoplastics, thermosets, hydrogels, other extrusion techniques. Moreover, diverse exhibited printed polymers, mechanical strength, conductance, self‐healing, well integrated are highlighted. Lastly, stimuli responsiveness polymeric materials shape morphing, degradability, color changing discussed.

Language: Английский

---

Mechano-responsive hydrogen-bonding array of thermoplastic polyurethane elastomer captures both strength and self-healing

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Jan. 27, 2021

Self-repairable materials strive to emulate curable and resilient biological tissue; however, their performance is currently insufficient for commercialization purposes because mending toughening are mutually exclusive. Herein, we report a carbonate-type thermoplastic polyurethane elastomer that self-heals at 35 °C exhibits tensile strength of 43 MPa; this as strong the soles used in footwear. Distinctively, it has abundant carbonyl groups soft-segments fully amorphous with negligible phase separation due poor hard-segment stacking. It operates dual mechano-responsive mode through reversible disorder-to-order transition its hydrogen-bonding array; heals when static toughens dynamic. In mode, non-crystalline hard segments promote dynamic exchange disordered hydrogen-bonds self-healing. The forms stiff crystals stretched orders inter-chain hydrogen bonding. strain return pre-stressed state after release repeat healing process.

Language: Английский

---

Intrinsically Self-Healing Polymers: From Mechanistic Insight to Current Challenges

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(2), P. 701 - 735

Published: Dec. 28, 2022

Self-healing materials open new prospects for more sustainable technologies with improved material performance and devices' longevity. We present an overview of the recent developments in field intrinsically self-healing polymers, broad class based mostly on polymers dynamic covalent noncovalent bonds. describe current models mechanisms discuss several examples systems different types bonds, from various hydrogen bonds to The advances indicate that most intriguing results are obtained have combined These demonstrate high toughness along a relatively fast rate. There is clear trade-off relationship between rate mechanical modulus materials, we propose design principles toward surpassing this trade-off. also applications summarize challenges field. This review intends provide guidance intrinsic required properties.

Language: Английский

---

A self-reinforcing and self-healing elastomer with high strength, unprecedented toughness and room-temperature reparability

Materials Horizons, Journal Year: 2020, Volume and Issue: 8(1), P. 267 - 275

Published: Nov. 2, 2020

The development of intrinsic self-healing elastomers with simultaneous high mechanical strength, toughness and room-temperature reparability remains a formidable challenge. Herein, we report mechano-responsive strategy, known as strain induced crystallization, to address the above issue, whereby synthesized unprecedented performances are bestowed materials, achieving tensile fracture energy values 29.0 MPa, 121.8 MJ m-3 104.1 kJ m-2, respectively.

Language: Английский

---