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Polymers · 2023 ·Vol. 15 ·期 3 ·724 · IF 5

Binary Double Network-like Structure: An Effective Energy-Dissipation System for Strong Tough Hydrogel Design

Genxin Chen,Sijie Tang,Honghan Yan,Xiongbin Zhu,Huimin Wang,Liya Ma,Kang Mao,Changying Yang,Jiabing Ran

Currently, hydrogels simultaneously featuring high strength, high toughness, superior recoverability, and benign anti-fatigue properties have demonstrated great application potential in broad fields; thus, great efforts have been made by researchers to develop satisfactory hydrogels. Inspired by the double network (DN)-like theory, we previously reported a novel high-strength/high-toughness hydrogel which had two consecutive energy-dissipation systems, namely, the unzipping of coordinate bonds and the dissociation of the crystalline network. However, this structural design greatly damaged its stretchability, toughness recoverability, shape recoverability, and anti-fatigue capability. Thus, we realized that a soft/ductile matrix is indispensable for an advanced strong tough hydrogel. On basis of our previous work, we herein reported a modified energy-dissipation model, namely, a “binary DN-like structure” for strong tough hydrogel design for the first time. This structural model comprises three interpenetrated polymer networks: a covalent/ionic dually crosslinked tightened polymer network (stiff, first order network), a constrictive crystalline polymer network (sub-stiff, second order network), and a ductile/flexible polymer network (soft, third order network). We hypothesized that under low tension, the first order network served as the sacrificing phase through decoordination of ionic crosslinks, while the second order and third order networks together functioned as the elastic matrix phase; under high tension, the second order network worked as the energy dissipation phase (ionic crosslinks have been destroyed at the time), while the third order network played the role of the elastic matrix phase. Owing to the “binary DN-like” structure, the as-prepared hydrogel, in principle, should demonstrate enhanced energy dissipation capability, toughness/shape recoverability, and anti-fatigue/anti-tearing capability. Finally, through a series of characterizations, the unique “binary DN-like” structure was proved to fit well with our initial theoretical assumption. Moreover, compared to other energy-dissipation models, this structural design showed a significant advantage regarding comprehensive properties. Therefore, we think this design philosophy would inspire the development of advanced strong tough hydrogel in the future.Keywords:double-network;hydrogel;toughness

CAS / MDL: 79-06-1
研究领域: 材料科学 · 生物工程
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA · 2025 ·Vol. 122 ·期 15 ·e2417978122 · IF 9.1

Glassy ionogels with high compressibility and strength for impact protection

Jiayu Wang,Shilong Zhang,Lingling Li,Xiaoliang Wang,Jiaofeng Xiong,Qingning Li,Weizheng Li,Feng Yan

Solvents within gels enhance the mobility of polymer chain segments while concurrently diminishing interchain interactions, thereby facilitating the ductility of glassy polymers at the cost of their mechanical strength. Here, we develop a solvent toughening strategy for the preparation of highly compressible and high-strength ionogels in the glassy state. This approach leverages the synergistic effects of the slow dissociation-shift kinetics of solvent ionic liquids and polymer crystallization. Ionogels exhibit an ultimate compressive stress of 2.3 GPa (at 98% compressive strain), toughness of 1219.3 MJ m−3, and energy dissipation rate of 81.9% (at 70% compression strain). The highly interacting ionic bonds of solvent and the fast crystallization of polymers under load toughen the ionogels and confer impact hardening and efficient energy dissipation behavior under fast impact. A 500-μm-thick ionogel coating can protect fragile items, such as glass, from impact damage. Ionogels, renowned for their impact resistance, hold promise for various applications across industries including human body implants, equipment, transportation, and aerospace.

研究领域: 材料科学 · 力学 · 工程学
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POLYMER COMPOSITES · 2025 · IF 4.7

A high dielectric damping material with flexibility, self-healing capability, reprocessing capability and impact resistance based on CaCu3Ti4O12/poly(lipoic acid)

Che Zhao,Yuxuan Zeng,Yuhan Zhou,Tianyu Wu,Meng Song,Lei Duan,Jiamei Dong,Yanlong Luo

Cross-linked polymeric damping materials with efficient energy dissipation mechanisms have attracted significant attention in impact protection applications. However, conventional viscoelastic damping materials frequently encounter limitations in processability and operational durability. Herein, a novel high-dielectric CaCu 3 Ti 4 O 12 /poly(lipoic acid) dynamic covalent network composite was introduced. This advanced material demonstrated an exceptional self-healing efficiency of 89.7% after 24 h at ambient temperature and remarkable reprocessability through thermally activated bond exchange reactions. Upon damage, the material's mechanical strength and integrity can be restored via the reformation of cross-linking points within the polymer network, thereby extending its operational lifespan. Notably, the synergistic combination of interfacial polarization effects from CaCu 3 Ti 4 O 12 particles and the dynamic equilibrium of coordination bonds establishes multiple energy dissipation pathways. This unique architecture achieves broadband damping performance with loss factors (tan δ) exceeding 0.3 across an extended frequency spectrum (0.009–100 Hz), coupled with a substantial enhancement in dielectric constant. The energy dissipation capability was verified through a steel ball rebound experiment, which demonstrated an exceptionally low rebound rate of 3.0%. This research offers an innovative design concept for developing sustainable impact-resistant materials. Highlights A novel high-dielectric self-healing CaCu 3 Ti 4 O 12 /poly(lipoic acid) damping material was successfully synthesized. The CaCu 3 Ti 4 O 12 /poly(lipoic acid) films exhibit outstanding self-healing ability and reprocessability. The CaCu 3 Ti 4 O 12 /poly(lipoic acid) composites achieve a superior impact resistance and a significantly elevated dielectric constant.

CAS / MDL: 1200-22-2
研究领域: 材料科学 · 高分子化学 · 力学
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Extreme Mechanics Letters · 2021 · IF 4.567

Switchable adhesion between hydrogels by wrinkling

Qi Li,Ping Zhang,Canhui Yang,Huiling Duan,Wei Hong

On-demand adhere to and detach from soft and wet surfaces are crucial for hydrogels for applications in tissue engineering , soft machines, and soft robotics. Whereas strong adhesion has been achieved between hydrogels, on-demand switching from strong adhesion to weak adhesion for benign detachment is still under explorations. Herein, we report an approach for switchable adhesion between hydrogels by invoking a mechanical process, wrinkling. The approach is demonstrated by bonding two hydrogel adherends with a wrinkled hydrogel adhesive , with the formation and characterizations of wrinkles tailored by regulating the prestretch of adherend and optimizing the ingredients of adhesive synergistically. On one hand, the formation of wrinkles enhances adhesion by creating a tortuous path for crack propagation and an extended energy dissipation zone. The resulting adhesion is robust to elicit bulk dissipation within the adherend and transform the once adhesive failure to cohesive failure . On the other hand, the suppression of wrinkles deactivates the adhesion enhancement mechanism to facilitate effortless debonding. As a proof-of-concept, a hydrogel patch that can strongly adhere to a damaged hydrogel device for repair and gently detach after repairing, based on the switchable hydrogel adhesion, is demonstrated. The proposed method expands the design space for hydrogel adhesion.

研究领域: 生物医学工程 · 材料科学 · 组织工程
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CONSTRUCTION AND BUILDING MATERIALS · 2019 · IF 4.046

Mechanical properties and constitutive models of foamed steels under monotonic and cyclic loading

Mingzhou Su,Qiaoling Zhou,Huimeng Wang

Foamed steel applications in civil engineering are at their beginning stage. Compared to foamed aluminum, advantages of using steel as a base metal are distinct (e.g., higher strength and modulus). In order to investigate the mechanical properties of foamed steels and to obtain representative material constitutive parameters for finite element analysis, fourteen specimens were tested under monotonic and eleven different cyclic loading schemes in this study. The monotonic and cyclic tensile-to-yield ratios were 2.17 and 1.90 ± 0.17, respectively, and the energy dissipation coefficient ranged from 2.70 to 3.35. The cyclic hardening behavior of foamed steels comprised isotropic and kinematic hardening characteristics, and the isotropic part played the dominate role. Based on the test results, the corresponding material parameters for two cyclic constitutive models, including the Chaboche model and the Giuffré-Menegotto-Pinto model were obtained. Then, the accuracy of the parameters was verified by nonlinear analysis results in ABAQUS and OpenSEES. This work may provide a valuable reference for further research into the cyclic characteristics of foamed steels.

研究领域: 土木工程 · 材料科学
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FUEL · 2023 · IF 7.4

Effect of Na+ on the collision of the dodecane droplet and kinetic energy transfer

Xiaojian Wei,Yong Zhang,Hongzheng Zhu,Ming Yang,Jinbo Zhu

Using a high-speed motion acquisition system, the dodecane droplet size and the interface energy of the dodecane-solution interface during the collision between the dodecane droplet and the dodecane layer at different Na + concentrations were studied. The collision process is divided into three stages: Contact stage , Stretch stage and Attenuation amplitude stage . The size of the dodecane droplet gradually decreases as the Na + concentration increases, and the stretching time does too. The kinetic energy of the dodecane droplet, the surface energy of the dodecane-solution interface, and the net force of the dodecane droplet all decrease with an increase in Na + concentration, but the dodecane droplet rate of energy dissipation increases. The effect of Na + concentration on dodecane-solution interfacial tension is the main reason for the collision difference. The Na + added to the solution forms a hydration shell around it, weakening the interaction between water molecules at the dodecane-solution interface and within the solution, leading to reduced interfacial tension. The advancement of mineral flotation technology may benefit greatly from these findings.

CAS / MDL: 7647-14-5
研究领域: 化学工程 · 表面科学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Tough double network hydrogels with rapid self-reinforcement and low hysteresis based on highly entangled networks

Zhu Ruixin,Zhu Dandan,Zheng Zhen,Wang Xinling

Most tough hydrogels are reinforced by introducing energy dissipation mechanisms, but simultaneously realizing a high toughness and low hysteresis is challenging because the energy dissipation structure cannot recover rapidly. In this work, high mechanical performance highly entangled double network hydrogels without energy dissipation structure are fabricated, in which physical entanglements act as the primary effective crosslinking in the first network. This sliding entanglement structure allows the hydrogel network to form a highly uniform oriented structure during stretching, resulting in a high tensile strength of ~3 MPa, a fracture energy of 8340 J m −2 and a strain-stiffening capability of 47.5 in 90% water content. Moreover, almost 100% reversibility is obtained in this hydrogel via energy storage based on entropy loss. The highly entangled double network structure not only overcomes the typical trade-off between the high toughness and low hysteresis of hydrogels, but more importantly, it provides an insight into the application of entanglement structures in high-performance hydrogels.

CAS / MDL: 79-10-7
研究领域: 材料科学 · 生物医学工程
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Design of high-energy-dissipation, deformable binder for high-areal-capacity silicon anode in lithium-ion batteries

Linlin Hu,Xudong Zhang,Bing Li,Mihan Jin,Xiaohui Shen,Zongwu Luo,Zhanyuan Tian,Lizhi Yuan,Junkai Deng,Zhengfei Dai,Jiangxuan Song

Although silicon has the highest theoretical capacity among the existing anode materials, its practical application is highly hindered by huge interface stress arising from large volume change upon cycling. Herein, an efficient energy-dissipation engineering was harnessed on high-capacity silicon anodes through a synergized “static” (chemically crosslinking) and “dynamic” (physically crosslinking) binder. In this dual network, the disassociation of non-covalent hydrogen bonds greatly facilitates the dispersion and release of unfavorable stress, while the permanent chemical bonding network enables a deformable network to sustain the electrode structure. Such a strategy effectively avoids both materials and electrodes deterioration and promises a better Si-based anode: a high areal capacity of 2 mAh cm −2 with capacity retention of 91.3% after 200 cycles. Meanwhile, the energy-dissipation mechanism was further clarified by temperature-dependent FTIR and finite element simulations.

研究领域: 材料科学 · 电化学 · 锂离子电池
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ADVANCED MATERIALS · 2020 ·Vol. 32 ·期 33 ·2001222 · IF 27.398

Bioinspired Multifunctional Cellular Plastics with a Negative Poisson’s Ratio for High Energy Dissipation

Dewen Li,Xiaochen Bu,Zongpu Xu,Yingwu Luo,Hao Bai

Cellular plastics have been widely used in transportation, aerospace, and personal safety applications owing to their excellent mechanical, thermal, and acoustic properties. It is highly desirable to impart them with a complex porous structure and composition distribution to obtain specific functionality for various engineering applications, which is challenging with conventional foaming technologies. Herein, it is demonstrated that this can be achieved through the controlled freezing process of a monomer/water emulsion, followed by cryopolymerization and room temperature thawing. As ice is used as a template, this method is environmentally friendly and capable of producing cellular plastics with various microstructures by harnessing the numerous morphologies of ice crystals. In particular, a cellular plastic with a radially aligned structure shows a negative Poisson’s ratio under compression. The rigid plastic shows a much higher energy dissipation capability compared to other materials with similar negative Poisson’s ratios. Additionally, the simplicity and scalability of this approach provides new possibilities for fabricating high-performance cellular plastics with well-defined porous structures and composition distributions.

研究领域: 材料科学 · 仿生学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Full Poly(ethylene glycol) Hydrogels with High Ductility and Self-Recoverability

Pengfei Ge,Qiuquan Cai,Hongjie Zhang,Xuxia Yao,Weipu Zhu

Energy dissipation is a common mechanism to improve the ductility of polymeric hydrogels. However, for poly(ethylene glycol) (PEG) hydrogels, it is not easy to dissipate energy, as polymer chains are dispersed in water without strong interchain interactions or decent entanglement. The brittleness limits the real applications of PEG hydrogels, although they are promising candidates in biomedical fields, as PEG has been approved by the U.S. Food and Drug Administration. Herein, we chemically introduced a center for energy dissipation in the PEG hydrogel system. Amphiphilic segmented PEG derivatives were designed through the melt polycondensation of triethylene glycol (PEG150) and high molecular weight PEG in the presence of succinic acid and mercaptosuccinic acid as dicarboxylic acids. Full PEG hydrogels with elastic nanospheres as giant cross-linkers were facilely prepared by the self-assembly of esterified PEG150 segments and the oxidation of mercapto groups. The resultant full PEG hydrogels can dissipate energy by the deformation of elastic nanospheres with outstanding ductility and self-recoverability while maintaining the excellent biocompatibility owing to their full PEG components. This work provides an original strategy to fabricate full PEG hydrogels with high ductility and self-recoverability, potentially applicable in biomedical fields.

研究领域: 材料科学 · 生物医学工程
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NEW JOURNAL OF CHEMISTRY · 2016 ·Vol. 40 ·期 10 ·8650-8657 · IF 3.277

Long-chain branching hydrogel with ultrahigh tensibility and high strength by grafting via photo-induced polymerization

Shuangfei Xiang,Ting Li,Yang Wang,Piming Ma,Mingqing Chen,Weifu Dong

A novel long-chain branching (LCB) hydrogel, polyacrylamide grafted from poly(2-acrylamido-2-methylpropanesulfonic acid) via photo-induced polymerization, has been developed with excellent mechanical properties such as ultrahigh tensibility and high strength. Investigations of tensile and compressive properties indicate that the Young's modulus, ultimate strength and strain, toughness, compressive modulus and stress are significantly improved by introduction of LCB. Scanning electron microscopy (SEM) reveals that the amount of embedded micro-network structures in LCB gels is increased with an increase in the length of LCB. The compressive loading–unloading behaviour shows that the area of the hysteresis loop (the dissipated energy) for the first compressive cycle increases with the introduction of LCB and is higher than that for subsequent cycles. The energy dissipation mechanism is demonstrated for a better understanding of LCB gels. Furthermore, rheological measurements are also studied. Dynamic shear measurements show that both the storage modulus and the complex viscosity increase in the presence of LCB.

研究领域: 材料科学 · 生物材料
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POLYMER TESTING · 2024 · IF 5

Experimental and numerical study on CuO/ZnO-modified aramid fabric for ballistic and UV radiation protection

li Liu,Fenglei Huang,Yaojie Xu,Xuke Lan,Guangyan Huang

Aramid fabrics are widely used in bulletproof armor because of their excellent mechanical properties. Previous studies have shown that ultraviolet radiation has a negative effect on the mechanical properties of aramid yarn, so improving the mechanical properties and impact resistance of aramid fabrics under ultraviolet radiation has become a research focus. In this work, aramid fabric was modified with CuO and ZnO particles to improve its ballistic performance under ultraviolet radiation. The ballistic impact resistance response and microscopic failure mechanisms of aramid fabrics under ultraviolet radiation were analyzed in detail. Under ultraviolet radiation, the ballistic limit velocity ( v bl ) of the CuO/ZnO-modified aramid fabric was 185.1 % greater than that of a neat fabric with a similar areal density. The v bl of the single-layer modified fabric was 45.6 % greater than that of the two-layer neat fabrics. The decrease in the ballistic performance of the aramid fabric under ultraviolet radiation was attributed to surface damage caused by the fracture of the chemical structure of the fibers, which weakened the mechanical properties of the fabric. The numerical simulation results were highly consistent with the ballistic impact test results, and the error between the numerical simulation and experimental results was within 10 %. The effects of changes in the mechanical parameters of the fabrics on the protection mechanism and energy absorption structure during ballistic impact were investigated. The energy dissipation of the modified fabric was at least 147.7 % greater than that of the neat fabric, further explaining the significant improvement in the ballistic performance of CuO/ZnO-modified fabrics under ultraviolet radiation.

研究领域: 材料科学 · 纺织工程 · 力学
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