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Polymers · 2023 ·Vol. 15 ·期 19 ·4020 · IF 5

Mechanical Robust, Self-Healable Polyurethane Elastomer Enabled by Hierarchical Hydrogen Bonds and Disulfide Bonds

Biqiang Jin,Wenqiang Wu,Haitao Wu

The fabrication of mechanically robust and self-healing polymeric materials remains a formidable challenge. To address the drawbacks, a core strategy is proposed based on the dynamic hard domains formed by hierarchical hydrogen bonds and disulfide bonds. The dynamic hard domains dissipate considerable stress energy during stretching. Meanwhile, the synergistic effect of hierarchical hydrogen bonds and disulfide bonds greatly enhances the relaxation dynamics of the PU network chains, thus accelerating network reorganization. Therefore, this designed strategy effectively solves the inherent drawback between cohesive energy and relaxation dynamics of the PU network. As a result, the PU elastomer has excellent mechanical properties (9.9 MPa and 44.87 MJ/m3) and high self-healing efficiency (96.2%). This approach provides a universal but valid strategy to fabricate high-performance self-healing polymeric materials. Meanwhile, such materials can be extended to emerging fields such as flexible robotics and wearable electronics.Keywords:polyurethane elastomer;hierarchical hydrogen bonds;disulfide bonds;mechanical robustness;self-healing

CAS / MDL: 25190-06-1
研究领域: 材料科学 · 化学工程
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ADVANCED MATERIALS · 2025 · IF 26.8

3D-Printing of Ultratough and Healable Elastomers

Hongfeng Mu,Zhuo Sun,Jiada Chen,Chenyue Xu,Xiaoyu Zhang,Xingqun Pu,Ning Zheng,Qian Zhao,Tao Xie,Jingjun Wu,Zizheng Fang

Although 3D-printing has offered a promising solution for the freeform fabrication of complex, arbitrary structures, developing elastomeric materials that simultaneously possess mechanical robustness and self-healing functionality remains a significant challenge. To address this, a 3D-printable elastomer is reported by the strategic incorporation of hierarchical hydrogen bonding (acylsemicarbazide and carbamate) into the photoactive resin, thereby overcoming the traditional trade-off between mechanical strength and dynamic functionality. The resulting elastomer exhibits ultra-toughness (158.5 MJ m −3 ), with tensile strength and breaking strain of 49.6 MPa and 1136%, respectively. In addition, the acylsemicarbazide moieties endow the 3D-printed elastomers with unique dynamic characteristics, including self-healing capabilities and shape reconfigurability, thus significantly enhancing the design flexibility and versatility of complex structures.

研究领域: 材料科学 · 高分子科学 · 机械工程 · 增材制造
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Materials Horizons · 2023 ·Vol. 10 ·期 10 ·4183-4191 · IF 13.3

A strain-reinforcing elastomer adhesive with superior adhesive strength and toughness

Chuanlong Li,Wenbo Dong,Longyu Li,Zhengli Dou,Yuhan Li,Liuhe Wei,Qin Zhang,Qiang Fu,Kai Wu

Strong and ductile adhesives often undergo both interfacial and cohesive failure during the debonding process. Herein, we report a rare self-reinforcing polyurethane adhesive that shows the different phenomenon of only interfacial failure yet still exhibiting superior adhesive strength and toughness. It is synthesized by designing a hanging adhesive moiety, hierarchical H-bond moieties, and a crystallizable soft segment into one macromolecular polyurethane. The former hanging adhesive moiety allows the hot-melt adhesive to effectively associate with the target substrate, providing sufficient adhesion energy; the latter hierarchical H-bond moieties and a crystallizable soft segment cooperate to enable the adhesive to undergo large lap-shear deformations through sacrificing weak bonds and mechano-responsive strength through the fundamental mechanism of strain-induced crystallization. As a result, this polyurethane adhesive can keep itself intact during the debonding process while still withstanding a high lap-shear strength and dissipating tremendous stress energy. Its adhesive strength and work of debonding are as high as 11.37 MPa and 10.32 kN m−1, respectively, outperforming most reported tough adhesives. This self-reinforcing adhesive is regarded as a new member of the family of strong and ductile adhesives, which will provide innovative chemical and structural inspirations for future conveniently detachable yet high-performance adhesives.

CAS / MDL: 4767-03-7 77-76-9
研究领域: 材料科学 · 高分子化学 · 胶粘技术
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

High Strength Polyurea Elastomers with Superior Room Temperature Self-Healing, Recyclability, and Extreme-Temperature Mechanical Robustness

Lin Wang,Yingdong Zhang,Zhiwei Yang,Manman Jia,Dongmei Yue

Achieving simultaneous high strength, toughness, room temperature self-healing, recyclability, and extreme-temperature adaptability remains a critical challenge for thermoplastic elastomers (TPE). Here, a series of thermoplastic polyurea elastomers (IPDI-D2000-PPD) with hierarchical hydrogen-bonding networks are synthesized using polyether amine (D2000) as soft segments, isophorone diisocyanate (IPDI) as hard segments, and p-phenylenediamine (PPD) as chain extenders. By adjusting hard-segment content, the materials exhibit outstanding room-temperature properties, including tensile strength up to 38.6 MPa, toughness reaching 164.2 MJ m −3 , true stress of 354.0 MPa, and remarkable crack tolerance, whereby the notched sample can lift 48,600 times its own weight. The synergistic effects of flexible polyether chains and reversible hydrogen bonds endow the elastomers with 90% self-healing efficiency at room temperature under trace ethanol and over 90% mechanical recovery after four recycling cycles. Importantly, they retain mechanical robustness across extreme temperatures, with strengths of 56.4 MPa at −50 °C and 14.3 MPa at 120 °C, and toughness of 143.6 and 98.6 MJ m −3 . Incorporation of ionic liquids further yields conductive ionogels for strain sensing. This work demonstrates a simple and versatile molecular design strategy, bridging performance gaps in multifunctional elastomers for sustainable, extreme-temperature adaptability, and intelligent applications.

CAS / MDL: 4098-71-9 9046-10-0
研究领域: 材料科学 · 高分子化学 · 智能材料 · 自修复材料 · 可持续材料
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Dolphins-inspired antifouling self-healing hydrophilic coatings with hierarchical hydrogen bonds for enhanced durability in antifouling performance based on dynamic poly(urethane-urea)

Yu Guan,Rongrong Chen,Jiahui Zhu,Gaohui Sun,Qi Liu,Jingyuan Liu,Jing Yu,Zailin Yang,Jun Wang

Hydrophilic coatings are widely used in marine antifouling. Nevertheless, there are additional requirements for the robustness of marine antifouling coatings, including the ability to withstand scratches and damage. Therefore, the demand for self-healing properties and robust mechanical strength is high, presenting significant challenges. Herein, inspired by the elastic surface and exceptional water absorption capabilities of dolphins, a reversible interlocking polymer network with multiple hydrogen bonds was successfully developed. This innovation harnesses the properties of poly(urethane-urea) and ureido pyrimidinone, thereby enhancing both mechanical properties and antifouling performance. Furthermore, the modified 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide was incorporated into the system as a functional filler and to serve as crosslinking points, creating a multifunctional coating. Owing to the hierarchical hydrogen bonds (the hydrogen-bonded carbonyl groups in SPPU-01 reach as high as 56.80 %), SPPU-01 exhibits exceptional strength of 17.35 MPa (1132.17 %), remarkable toughness of 89.33 MJ/m 3 , and superior tear strength of 74.97 KN/m. Upon incorporating additional components, the composite crosslinking network enhances hydrophilicity (∼29.15°), thereby forming a hydration layer that effectively prevents fouling. The SPPU-02 reveals outstanding resistance to marine bacteria, effective anti-diatom adhesion, robust anti-mussel attachment, and strong anti-pseudo-barnacle properties, achieving 96.5 %, 94.5 %, 96.04 %, and 1.31 MPa, respectively. Furthermore, this strategy, which mimics dolphin functions, is well-suited for various marine materials with different requirements. It exhibits deicing (21.22 kPa), drag reduction, and high-temperature resistance properties (69.1 %), opening new avenues for the development of antifouling coatings with both strong and superior comprehensive performance.

CAS / MDL: 109-66-0 77-58-7
研究领域: 海洋涂层 · 材料科学 · 仿生学 · 高分子科学 · 表面工程 · 防污技术
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Advanced Science · 2024 ·Vol. 11 ·期 35 ·2405301 · IF 14.3

Sustainable Plastics with High Performance and Convenient Processibility

Guogang Xu,Lei Hou,Peiyi Wu

Designing and making sustainable plastics is especially urgent to reduce their ecological and environmental impacts. However, it remains challenging to construct plastics with simultaneous high sustainability and outstanding comprehensive performance. Here, a composite strategy of in situ polymerizing a petroleum-based monomer with the presence of an industrialized bio-derived polymer in a quasi-solvent-free system is introduced, affording the plastic with excellent mechanical robustness, impressive thermal and solvent stability, as well as low energy, consumes during production, processing, and recycling. Particularly, the plastic can be easily processed into diverse shapes through 3D printing, injection molding, etc. during polymerization and further reprocessed into other complex structures via eco-friendly hydrosetting. In addition, the plastic is mechanically robust with Young's modulus of up to 3.7 GPa and tensile breaking strength of up to 150.2 MPa, superior to many commercially available plastics and other sustainable plastics. It is revealed that hierarchical hydrogen bonds in plastic predominate the well-balanced sustainability and performance. This work provides a new path for fabricating high-performance sustainable plastic toward practical applications, contributing to the circular economy.

CAS / MDL: 9004-65-3 7473-98-5
研究领域: 材料科学 · 高分子科学 · 可持续性 · 环境科学 · 化学工程
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