Molecular mechanism of abnormally large nonsoftening deformation in a tough hydrogel.

Published on Apr 6, 2021in Proceedings of the National Academy of Sciences of the United States of America11.205
· DOI :10.1073/PNAS.2014694118
Ya Nan Ye7
Estimated H-index: 7
(Hokkaido University),
Kunpeng Cui22
Estimated H-index: 22
(Hokkaido University)
+ 6 AuthorsJian Ping Gong81
Estimated H-index: 81
(Hokkaido University)
Sources
Abstract
Tough soft materials usually show strain softening and inelastic deformation. Here, we study the molecular mechanism of abnormally large nonsoftening, quasi-linear but inelastic deformation in tough hydrogels made of hyperconnective physical network and linear polymers as molecular glues to the network. The interplay of hyperconnectivity of network and effective load transfer by molecular glues prevents stress concentration, which is revealed by an affine deformation of the network to the bulk deformation up to sample failure. The suppression of local stress concentration and strain amplification plays a key role in avoiding necking or strain softening and endows the gels with a unique large nonsoftening, quasi-linear but inelastic deformation.
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#1Kazuki Fukao (Hokkaido University)H-Index: 4
#2Tasuku Nakajima (Hokkaido University)H-Index: 37
Last. Jian Ping Gong (Hokkaido University)H-Index: 81
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Double network hydrogels (DN gels) exhibit extraordinarily high strength and toughness by interplay of the two contrasting networks: the rigid, brittle network serves as a sacrificial bond that fractures at a relatively low strain, while the soft, stretchable network serves as hidden length that sustains stress by large extension afterward. The internal fracture process of the brittle network strongly depends on the relative strength of the two networks. In this study, we study the internal frac...
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#1Xiaojian Liao (University of Bayreuth)H-Index: 9
#2Martin Dulle (Forschungszentrum Jülich)H-Index: 18
Last. Andreas Greiner (University of Bayreuth)H-Index: 81
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In materials science, there is an intrinsic conflict between high strength and high toughness, which can be resolved for different materials only through the use of innovative design principles. Advanced materials must be highly resistant to both deformation and fracture. We overcome this conflict in man-made polymer fibers and show multifibrillar polyacrylonitrile yarn with a toughness of 137 ± 21 joules per gram in combination with a tensile strength of 1236 ± 40 megapascals. The nearly perfec...
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#1Li Tang (University of Akron)H-Index: 3
#2Dong Zhang (University of Akron)H-Index: 30
Last. Jie Zheng (University of Akron)H-Index: 65
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Development of mechanically strong and adhesive hydrogels with self-recovery and self-healing properties is important for many applications but has proven to be very challenging. Here, we reported a double-network design strategy to synthesize a fully physically cross-linked double-network (DN) hydrogel, consisting of the first gelatin network and the second poly(N-hydroxyethyl acrylamide) network where both networks were mainly cross-linked by hydrogen bonds. The resultant gelatin/pHEAA hydroge...
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#2Kunpeng CuiH-Index: 22
Last. Jian Ping GongH-Index: 81
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We report a novel thermally responsive system from poly(butyl methacrylate)-b-poly(methacrylic acid)-b-poly(butyl methacrylate) (PBMA-b-PMAA-b-PBMA) triblock copolymer in dimethylformamide (DMF) solvent. This system shows a sol–gel transition by cooling below a critical temperature Tc. The network relaxation times of these gels rightly fall in the typical rheological experiment window, permitting us to investigate the relaxation dynamics and underlying mechanism, with a combination of linear rhe...
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#1Zhen Jiang (ANU: Australian National University)H-Index: 19
#2Broden Diggle (ANU: Australian National University)H-Index: 3
Last. Luke A. Connal (ANU: Australian National University)H-Index: 35
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: Achieving multifunctional shape-changing hydrogels with synergistic and engineered material properties is highly desirable for their expanding applications, yet remains an ongoing challenge. The synergistic design of multiple dynamic chemistries enables new directions for the development of such materials. Herein, a molecular design strategy is proposed based on a hydrogel combining acid-ether hydrogen bonding and imine bonds. This approach utilizes simple and scalable chemistries to produce a...
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Recent studies reported a multiscale structure in tough and self-healing hydrogels containing physical associations. For example, a type of tough and self-healing hydrogel from charge-balanced polyampholytes (PA) has a mesoscale bicontinuous double network structure with structural length around 400 nm. This mesoscale network structure plays an essential role in the multistep rupture process, which leads to the high toughness of PA hydrogels. In this work, by using an osmotic stress method, we s...
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#1Zbigniew Bartczak (PAN: Polish Academy of Sciences)H-Index: 29
#2Alina Vozniak (PAN: Polish Academy of Sciences)H-Index: 3
Abstract The influence of the topology of the amorphous phase on deformation instabilities, leading to kinking and to fragmentation of lamellae is discussed. Samples of polyethylene of diverse structure were deformed in the plane-strain compression. The accompanying structural changes were analyzed using DSC, WAXS and SAXS. Several deformation instabilities occur at various true strains. At e = 0.3–0.4 lamellae oriented specifically along the loading direction undergo microbuckling instability, ...
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#1Yunya Zhang (UVA: University of Virginia)H-Index: 17
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Nature’s wisdom resides in achieving a joint enhancement of strength and toughness by constructing intelligent, hierarchical architectures from extremely limited resources. A representative example is nacre, in which a brick-and-mortar structure enables a confluence of toughening mechanisms on multiple length scales. The result is an outstanding combination of strength and toughness which is hardly achieved by engineering materials. Here, a bioinspired Ni/Ni 3 C composite with nacre-like, brick-...
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: Understanding the energy dissipation mechanism during deformation is essential for the design and application of tough soft materials. We show that, in a class of tough and self-healing polyampholyte hydrogels, a bicontinuous network structure, consisting of a hard network and a soft network, is formed, independently of the chemical details of the hydrogels. Multiscale internal rupture processes, in which the double-network effect plays an important role, are found to be responsible for the la...
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#1Itamar Kolvin (HUJI: Hebrew University of Jerusalem)H-Index: 7
#2John Martin Kolinski (HUJI: Hebrew University of Jerusalem)H-Index: 7
Last. Jay Fineberg (HUJI: Hebrew University of Jerusalem)H-Index: 46
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Fracture of highly stretched materials challenges our view of how things break. We directly visualize rupture of tough double-network (DN) gels at >50\% strain. During fracture, crack tip shapes obey a x\sim y^{1.6}power-law, in contrast to the parabolic profile observed in low-strain cracks. A new length-scale \ellemerges from the power-law; we show that \ellscales directly with the stored elastic energy, and diverges when the crack velocity approaches the shear wave speed. Our results...
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Strength and toughness are usually mutually exclusive for materials. The sacrificial bond strategy is used to address the trade-off between strength and toughness. However, the complex construction process of sacrificial network limits the application of sacrificial network. This work develops a facile strategy to construct an interfacial interactions-driven sacrificial network. The authors' group finds that there are the interfacial interactions between arginines (A) aggregates and molecular ch...
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The intrinsic conflicts between mechanical performances and processability are main challenges to develop cost-effective impact-resistant materials from polymers and their composites. Herein, polyhedral oligomeric silsesquioxanes (POSSs) are integrated as side chains to the polymer backbones. The one-dimension (1D) rigid topology imposes strong space confinements to realize synergistic interactions among POSS units, reinforcing the correlations among polymer chains. The afforded composites demon...
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