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1

Wang, Jilong, Junhua Wei, and Jingjing Qiu. "Facile Synthesis of Tough Double Network Hydrogel." MRS Advances 1, no. 27 (2016): 1953–58. http://dx.doi.org/10.1557/adv.2016.127.

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ABSTRACTIn this paper, a facile and novel method was developed to fabricate high toughness and stiffness double network hydrogels made of ionical-linked natural hydrogel and synthetic hydrogel. The synthetic hydrogel network is formed firstly, and then the gel is soaked in the ionic solution to build second network to form double network hydrogel with high toughness and stiffness. Two different natural polymers, alginate and chitosan, are employed to build rigid and brittle network and poly(acrylamide) is used as soft network in double network hydrogel. The compressive strength of Calcium alginate/poly(acrylamide) double network hydrogels is increased twice than that of poly(acrylamide) single network hydrogels, and the Ca2+ ionically cross-linked alginate is the key to improve the compressive property of double network hydrogels as a sacrificial bond. However, the chitosan/poly(acrylamide) double network hydrogels exhibit no enhancement of compressive strength comparing to poly(acrylamide) single network hydrogels.
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2

Fu, Jun, Guorong Gao, and Yuanna Sun. "Non-covalent Tough Hydrogels for Functional Actuators." MRS Advances 1, no. 8 (2015): 501–7. http://dx.doi.org/10.1557/adv.2015.3.

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ABSTRACTTough and responsive hydrogels have recently attracted great research interests for potential applications in artifical muscles, soft robotics, and actuators, etc. This paper overviews our recent progresses in the design and synthesis of hydrogels with very high strength and toughness, and actuators based on these hydrogels. Inorganic nanospheres, nanorods, and nanosheets are exploited as multi-functional crosslinkers to adsorb or bond with hydrophilic chains, leading to hydrogels with very high strength, toughness, fatigue resistance, and/or self-healing. Introduction of functional groups including ionic monomers and amino groups results in hydrogels reponsive to pH, ionic strength and electric field. Besides, ionoprinting has been used to change local crosslink density based on reversible chelating/decomposition of metal ions with functional groups. This process is rapid and thus enables reversible and rapid actuation of hydrogel devices. Our studies will further aim to develop sophiscated devices by assembling hydrogel actuators.
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3

King, Daniel R., Tao Lin Sun, Yiwan Huang, et al. "Extremely tough composites from fabric reinforced polyampholyte hydrogels." Materials Horizons 2, no. 6 (2015): 584–91. http://dx.doi.org/10.1039/c5mh00127g.

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4

Wen, Jie, Xiaopeng Zhang, Mingwang Pan, Jinfeng Yuan, Zhanyu Jia, and Lei Zhu. "A Robust, Tough and Multifunctional Polyurethane/Tannic Acid Hydrogel Fabricated by Physical-Chemical Dual Crosslinking." Polymers 12, no. 1 (2020): 239. http://dx.doi.org/10.3390/polym12010239.

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Commonly synthetic polyethylene glycol polyurethane (PEG–PU) hydrogels possess poor mechanical properties, such as robustness and toughness, which limits their load-bearing application. Hence, it remains a challenge to prepare PEG–PU hydrogels with excellent mechanical properties. Herein, a novel double-crosslinked (DC) PEG–PU hydrogel was fabricated by combining chemical with physical crosslinking, where trimethylolpropane (TMP) was used as the first chemical crosslinker and polyphenol compound tannic acid (TA) was introduced into the single crosslinked PU network by simple immersion process. The second physical crosslinking was formed by numerous hydrogen bonds between urethane groups of PU and phenol hydroxyl groups in TA, which can endow PEG–PU hydrogel with good mechanical properties, self-recovery and a self-healing capability. The research results indicated that as little as a 30 mg·mL−1 TA solution enhanced the tensile strength and fracture energy of PEG–PU hydrogel from 0.27 to 2.2 MPa, 2.0 to 9.6 KJ·m−2, respectively. Moreover, the DC PEG–PU hydrogel possessed good adhesiveness to diverse substrates because of TA abundant catechol groups. This work shows a simple and versatile method to prepare a multifunctional DC single network PEG–PU hydrogel with excellent mechanical properties, and is expected to facilitate developments in the biomedical field.
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5

Furukawa, Hidemitsu, and Jian Ping Gong. "Tough Hydrogel - Learn from Nature." Advances in Science and Technology 61 (September 2008): 40–45. http://dx.doi.org/10.4028/www.scientific.net/ast.61.40.

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Gel is a fascinating material for its unique properties, such as phase-transition, chemomechanical behavior, stimuli-responsiveness, low surface sliding friction, and for its possible wide application in many industry fields. Recently, hydrogels have drawn special attraction in biological field due to its possible applications as soft man-made tissues. However, conventional hydrogels, especially polyelectrolyte gels, are mechanically too weak to be practically used in any stress or strain bearing applications. Inspired by the structure of articular cartilage, we discovered a general method to obtain very strong polyelectrolyte hydrogels containing 60-90% water by inducing a double-network (DN) structure for various combinations of hydrophilic polymers. The soft and wet gel materials with both a high strength and an extremely low surface friction would find wide applications not only in industry but also in biomedical field, for example, as substitutes of articular cartilage or other bio-tissues.
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6

Zhang, Yu, You Yong, Duo An, et al. "A drip-crosslinked tough hydrogel." Polymer 135 (January 2018): 327–30. http://dx.doi.org/10.1016/j.polymer.2017.12.036.

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7

Wei, Junhua, Jilong Wang, Siheng Su, Molla Hasan, Jingjing Qiu, and Shiren Wang. "A shape healable tough hydrogel." New Journal of Chemistry 39, no. 11 (2015): 8461–66. http://dx.doi.org/10.1039/c5nj01250c.

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8

Liu, Chunlin, Hui Jie Zhang, Xiangyu You, Kunpeng Cui, and Xuechuan Wang. "Electrically Conductive Tough Gelatin Hydrogel." Advanced Electronic Materials 6, no. 4 (2020): 2000040. http://dx.doi.org/10.1002/aelm.202000040.

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9

Javadi, Mohammad, Qi Gu, Sina Naficy, et al. "Conductive Tough Hydrogel for Bioapplications." Macromolecular Bioscience 18, no. 2 (2017): 1700270. http://dx.doi.org/10.1002/mabi.201700270.

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10

Jiang, Zhiqiang, Ya Li, Yirui Shen, et al. "Robust Hydrogel Adhesive with Dual Hydrogen Bond Networks." Molecules 26, no. 9 (2021): 2688. http://dx.doi.org/10.3390/molecules26092688.

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Hydrogel adhesives are attractive for applications in intelligent soft materials and tissue engineering, but conventional hydrogels usually have poor adhesion. In this study, we designed a strategy to synthesize a novel adhesive with a thin hydrogel adhesive layer integrated on a tough substrate hydrogel. The adhesive layer with positive charges of ammonium groups on the polymer backbones strongly bonds to a wide range of nonporous materials’ surfaces. The substrate layer with a dual hydrogen bond system consists of (i) weak hydrogen bonds between N,N-dimethyl acrylamide (DMAA) and acrylic acid (AAc) units and (ii) strong multiple hydrogen bonds between 2-ureido-4[1H]-pyrimidinone (UPy) units. The dual hydrogen-bond network endowed the hydrogel adhesives with unique mechanical properties, e.g., toughness, highly stretchability, and insensitivity to notches. The hydrogel adhesion to four types of materials like glass, 316L stainless steel, aluminum, Al2O3 ceramic, and two biological tissues including pig skin and pig kidney was investigated. The hydrogel bonds strongly to dry solid surfaces and wet tissue, which is promising for biomedical applications.
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11

Naficy, Sina, Hugh R. Brown, Joselito M. Razal, Geoffrey M. Spinks, and Philip G. Whitten. "Progress Toward Robust Polymer Hydrogels." Australian Journal of Chemistry 64, no. 8 (2011): 1007. http://dx.doi.org/10.1071/ch11156.

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In this review we highlight new developments in tough hydrogel materials in terms of their enhanced mechanical performance and their corresponding toughening mechanisms. These mechanically robust hydrogels have been developed over the past 10 years with many now showing mechanical properties comparable with those of natural tissues. By first reviewing the brittleness of conventional synthetic hydrogels, we introduce each new class of tough hydrogel: homogeneous gels, slip-link gels, double-network gels, nanocomposite gels and gels formed using poly-functional crosslinkers. In each case we provide a description of the fracture process that may be occurring. With the exception of double network gels where the enhanced toughness is quite well understood, these descriptions remain to be confirmed. We also introduce material property charts for conventional and tough synthetic hydrogels to illustrate the wide range of mechanical and swelling properties exhibited by these materials and to highlight links between these properties and the network topology. Finally, we provide some suggestions for further work particularly with regard to some unanswered questions and possible avenues for further enhancement of gel toughness.
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12

Yu, Kunhao, Di Wang, and Qiming Wang. "Tough and Self-Healable Nanocomposite Hydrogels for Repeatable Water Treatment." Polymers 10, no. 8 (2018): 880. http://dx.doi.org/10.3390/polym10080880.

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Nanomaterials with ultrahigh specific surface areas are promising adsorbents for water-pollutants such as dyes and heavy metal ions. However, an ongoing challenge is that the dispersed nanomaterials can easily flow into the water stream and induce secondary pollution. To address this challenge, we employed nanomaterials to bridge hydrogel networks to form a nanocomposite hydrogel as an alternative water-pollutant adsorbent. While most of the existing hydrogels that are used to treat wastewater are weak and non-healable, we present a tough TiO2 nanocomposite hydrogel that can be activated by ultraviolet (UV) light to demonstrate highly efficient self-healing, heavy metal adsorption, and repeatable dye degradation. The high toughness of the nanocomposite hydrogel is induced by the sequential detachment of polymer chains from the nanoparticle crosslinkers to dissipate the stored strain energy within the polymer network. The self-healing behavior is enabled by the UV-assisted rebinding of the reversible bonds between the polymer chains and nanoparticle surfaces. Also, the UV-induced free radicals on the TiO2 nanoparticle can facilitate the binding of heavy metal ions and repeated degradation of dye molecules. We expect this self-healable, photo-responsive, tough hydrogel to open various avenues for resilient and reusable wastewater treatment materials.
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13

Shin, Min Kyoon, Sun I. Kim, Seon Jeong Kim, et al. "A tough nanofiber hydrogel incorporating ferritin." Applied Physics Letters 93, no. 16 (2008): 163902. http://dx.doi.org/10.1063/1.3005596.

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14

Xu, Liju, Chen Wang, Yang Cui, Ailing Li, Yan Qiao, and Dong Qiu. "Conjoined-network rendered stiff and tough hydrogels from biogenic molecules." Science Advances 5, no. 2 (2019): eaau3442. http://dx.doi.org/10.1126/sciadv.aau3442.

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Hydrogels from biological sources are expected as potential structural biomaterials, but most of them are either soft or fragile. Here, a new strategy was developed to construct hydrogels that were both stiff and tough via the formation of the conjoined-network, which was distinct from improving homogeneity or incorporating energy dissipation mechanisms (double-network) approaches. Conjoined-network hydrogels stand for a class of hydrogels consisting of two or more networks that are connected by sharing interconnection points to collaborate and featured as follows: (i) All the composed networks had a similar or equal energy dissipation mechanism, and (ii) these networks were intertwined to effectively distribute stress in the whole system. As a specific example, a biogenic conjoined-network hydrogel was prepared by electrostatically cross-linking the chitosan-gelatin composite with multivalent sodium phytate. The combination of high compressive modulus and toughness was realized at the same time in the chitosan-gelatin-phytate system. Moreover, these physical hydrogels exhibited extraordinary self-recovery and fatigue resistance ability. Our results provide a general strategy for the design of biocompatible stiff and tough conjoined-network hydrogels due to a variety of potential cross-linking mechanisms available (e.g., electrostatic attraction, host-guest interaction, and hydrogen bonding).
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15

Xing, Wenjin, Amin Jamshidi Ghahfarokhi, Chaoming Xie, Sanaz Naghibi, Jonathan A. Campbell, and Youhong Tang. "Mechanical Properties of a Supramolecular Nanocomposite Hydrogel Containing Hydroxyl Groups Enriched Hyper-Branched Polymers." Polymers 13, no. 5 (2021): 805. http://dx.doi.org/10.3390/polym13050805.

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Owing to highly tunable topology and functional groups, hyper-branched polymers are a potential candidate for toughening agents, for achieving supramolecular interactions with hydrogel networks. However, their toughening effects and mechanisms are not well understood. Here, by means of tensile and pure shear testings, we characterise the mechanics of a nanoparticle–hydrogel hybrid system that incorporates a hyper-branched polymer (HBP) with abundant hydroxyl end groups into the matrix of the polyacrylic acid (PAA) hydrogel. We found that the third and fourth generations of HBP are more effective than the second one in terms of strengthening and toughening effects. At a HBP content of 14 wt%, compared to that of the pure PAA hydrogel, strengths of the hybrid hydrogels with the third and fourth HBPs are 2.3 and 2.5 times; toughnesses are increased by 525% and 820%. However, for the second generation, strength is little improved, and toughness is increased by 225%. It was found that the stiffness of the hybrid hydrogel is almost unchanged relative to that of the PAA hydrogel, evidencing the weak characteristic of hydrogen bonds in this system. In addition, an outstanding self-healing feature was observed, confirming the fast reforming nature of broken hydrogen bonds. For the hybrid hydrogel, the critical size of failure zone around the crack tip, where serious viscous dissipation occurs, is related to a fractocohesive length, being about 0.62 mm, one order of magnitude less than that of other tough double-network hydrogels. This study can promote the application of hyper-branched polymers in the rapid evolving field of hydrogels for improved performance.
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16

Wei, Junhua, Jilong Wang, Siheng Su, et al. "3D printing of an extremely tough hydrogel." RSC Advances 5, no. 99 (2015): 81324–29. http://dx.doi.org/10.1039/c5ra16362e.

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17

Bui, Hoang Linh, and Chun-Jen Huang. "Tough Polyelectrolyte Hydrogels with Antimicrobial Property via Incorporation of Natural Multivalent Phytic Acid." Polymers 11, no. 10 (2019): 1721. http://dx.doi.org/10.3390/polym11101721.

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Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding a chemical crosslinker and docking a physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits compressive stress of >1 MPa, along with high elasticity and fatigue-resistant properties. The enhanced mechanical properties of pTMAEMA-PA stem from the multivalent ion effect of PA via the formation of ion bridges within polyelectrolytes. In addition, a comparative study for a series of pTMAEMA-counterion complexes was conducted to elaborate the relationship between swelling ratio and mechanical strength. The study also revealed secondary factors, such as ion valency, ion specificity and hydrogen bond formation, holding crucial roles in tuning mechanical properties of the polyelectrolyte hydrogel. Furthermore, in bacteria attachment and disk diffusion tests, pTMAEMA-PA exhibits superior fouling resistance and antibacterial capability. The results reflect the fact that PA enables chelating strongly with divalent metal ions, hence, disrupting the outer membrane of bacteria, as well as dysfunction of organelles, DNA and protein. Overall, the work demonstrated a novel strategy for preparation of tough polyelectrolyte with antibacterial capability via docking PA to open up the potential use of PA in medical application.
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18

Song, Meng-Meng, Ya-Min Wang, Bing Wang, et al. "Super Tough, Ultrastretchable Hydrogel with Multistimuli Responsiveness." ACS Applied Materials & Interfaces 10, no. 17 (2018): 15021–29. http://dx.doi.org/10.1021/acsami.8b01410.

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19

Wu, Zhiying, Ping Zhang, Haihui Zhang, et al. "Tough porous nanocomposite hydrogel for water treatment." Journal of Hazardous Materials 421 (January 2022): 126754. http://dx.doi.org/10.1016/j.jhazmat.2021.126754.

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20

Hua, Yujie, Huitang Xia, Litao Jia, et al. "Ultrafast, tough, and adhesive hydrogel based on hybrid photocrosslinking for articular cartilage repair in water-filled arthroscopy." Science Advances 7, no. 35 (2021): eabg0628. http://dx.doi.org/10.1126/sciadv.abg0628.

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A hydrogel scaffold for direct tissue-engineering application in water-irrigated, arthroscopic cartilage repair, is badly needed. However, such hydrogels must cure quickly under water, bind strongly and permanently to the surrounding tissue, and maintain sufficient mechanical strength to withstand the hydraulic pressure of arthroscopic irrigation (~10 kilopascal). To address these challenges, we report a versatile hybrid photocrosslinkable (HPC) hydrogel fabricated though a combination of photoinitiated radical polymerization and photoinduced imine cross-linking. The ultrafast gelation, high mechanical strength, and strong adhesion to native tissue enable the direct use of these hydrogels in irrigated arthroscopic treatments. We demonstrate, through in vivo articular cartilage defect repair in the weight-bearing regions of swine models, that the HPC hydrogel can serve as an arthroscopic autologous chondrocyte implantation scaffold for long-term cartilage regeneration, integration, and reconstruction of articular function.
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21

Milovanovic, Marko, Lydia Mihailowitsch, Mathusiha Santhirasegaran, Volker Brandt, and Joerg C. Tiller. "Enzyme-induced mineralization of hydrogels with amorphous calcium carbonate for fast synthesis of ultrastiff, strong and tough organic–inorganic double networks." Journal of Materials Science 56, no. 27 (2021): 15299–312. http://dx.doi.org/10.1007/s10853-021-06204-6.

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Abstract Hydrogels with good mechanical properties have great importance in biological and medical applications. Double-network (DN) hydrogels were found to be very tough materials. If one of the two network phases is an inorganic material, the DN hydrogels also become very stiff without losing their toughness. So far, the only example of such an organic–inorganic DN hydrogel is based on calcium phosphate, which takes about a week to be formed as an amorphous inorganic phase by enzyme-induced mineralization. An alternative organic–inorganic DN hydrogel, based on amorphous CaCO3, which can be formed as inorganic phase within hours, was designed in this study. The precipitation of CaCO3 within a hydrogel was induced by urease and a urea/CaCl2 calcification medium. The amorphous character of the CaCO3 was retained by using the previously reported crystallization inhibiting effects of N-(phosphonomethyl)glycine (PMGly). The connection between organic and inorganic phases via reversible bonds was realized by the introduction of ionic groups. The best results were obtained by copolymerization of acrylamide (AAm) and sodium acrylate (SA), which led to water-swollen organic–inorganic DN hydrogels with a high Young’s modulus (455 ± 80 MPa), remarkable tensile strength (3.4 ± 0.7 MPa) and fracture toughness (1.1 ± 0.2 kJ m−2). Graphical Abstract The present manuscript describes the method of enzymatic mineralization of hydrogels for the production of ultrastiff and strong composite hydrogels. By forming a double-network structure based on an organic and an inorganic phase, it is possible to improve the mechanical properties of a hydrogel, such as stiffness and strength, by several orders of magnitude. The key to this is the formation of a percolating, amorphous inorganic phase, which is achieved by inhibiting crystallization of precipitated amorphous CaCO3 with N-(phosphonomethyl)glycine and controlling the nanostructure with co polymerized sodium acrylate. This creates ultrastiff, strong and tough organic–inorganic double-network hydrogels.
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22

Xu, Bo, Yuwei Liu, Lanlan Wang, et al. "High-Strength Nanocomposite Hydrogels with Swelling-Resistant and Anti-Dehydration Properties." Polymers 10, no. 9 (2018): 1025. http://dx.doi.org/10.3390/polym10091025.

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Hydrogels with excellent mechanical properties have potential for use in various fields. However, the swelling of hydrogels under water and the dehydration of hydrogels in air severely limits the practical applications of high-strength hydrogels due to the influence of air and water on the mechanical performance of hydrogels. In this study, we report on a kind of tough and strong nanocomposite hydrogels (NC-G gels) with both swelling-resistant and anti-dehydration properties via in situ free radical copolymerization of acrylic acid (AA) and N-vinyl-2-pyrrolidone (VP) in the water-glycerol bi-solvent solutions containing small amounts of alumina nanoparticles (Al2O3 NPs) as the inorganic cross-linking agents. The topotactic chelation reactions between Al2O3 NPs and polymer matrix are thought to contribute to the cross-linking structure, outstanding mechanical performance, and swelling-resistant property of NC-G gels, whereas the strong hydrogen bonds between water and glycerol endow them with anti-dehydration capacity. As a result, the NC-G gels could maintain mechanical properties comparable to other as-prepared high-strength hydrogels when utilized both under water and in air environments. Thus, this novel type of hydrogel would considerably enlarge the application range of hydrogel materials.
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23

Nonoyama, Takayuki, and Jian Ping Gong. "Tough Double Network Hydrogel and Its Biomedical Applications." Annual Review of Chemical and Biomolecular Engineering 12, no. 1 (2021): 393–410. http://dx.doi.org/10.1146/annurev-chembioeng-101220-080338.

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Soft and wet hydrogels have many similarities to biological tissues, though their mechanical fragility had been one of the biggest obstacles in biomedical applications. Studies and developments in double network (DN) hydrogels have elucidated how to create tough gels universally based on sacrificial bond principles and opened a path for biomedical application of hydrogels in regenerative medicine and artificial soft connective tissues, such as cartilage, tendon, and ligament, which endure high tension and compression. This review explores a universal toughening mechanism for and biomedical studies of DN hydrogels. Moreover, because the term sacrificial bonds has been mentioned often in studies of bone tissues, consisting of biomacromolecules and biominerals, recent studies of gel–biomineral composites to understand early-stage osteogenesis and to simulate bony sacrificial bonds are also summarized.
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24

Teng, Wenqi, Thomas J. Long, Qianru Zhang, Ke Yao, Tueng T. Shen, and Buddy D. Ratner. "A tough, precision-porous hydrogel scaffold: Ophthalmologic applications." Biomaterials 35, no. 32 (2014): 8916–26. http://dx.doi.org/10.1016/j.biomaterials.2014.07.013.

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25

Zhu, Feng-bo, Hai-chao Yu, Wen-xi Lei, et al. "Tough polyion complex hydrogel films of natural polysaccharides." Chinese Journal of Polymer Science 35, no. 10 (2017): 1276–85. http://dx.doi.org/10.1007/s10118-017-1977-7.

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26

Xu, Xiuru, Chubin He, Feng Luo, Hao Wang, and Zhengchun Peng. "Transparent, Conductive Hydrogels with High Mechanical Strength and Toughness." Polymers 13, no. 12 (2021): 2004. http://dx.doi.org/10.3390/polym13122004.

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Transparent, conductive hydrogels with good mechanical strength and toughness are in great demand of the fields of biomedical and future wearable smart electronics. We reported a carboxymethyl chitosan (CMCS)–calcium chloride (CaCl2)/polyacrylamide (PAAm)/poly(N-methylol acrylamide (PNMA) transparent, tough and conductive hydrogel containing a bi-physical crosslinking network through in situ free radical polymerization. It showed excellent light transmittance (>90%), excellent toughness (10.72 MJ/m3), good tensile strength (at break, 2.65 MPa), breaking strain (707%), and high elastic modulus (0.30 MPa). The strain sensing performance is found with high sensitivity (maximum gauge factor 9.18, 0.5% detection limit), wide strain response range, fast response and recovery time, nearly zero hysteresis and good repeatability. This study extends the transparent, tough, conductive hydrogels to provide body-surface wearable devices that can accurately and repeatedly monitor the movement of body joints, including the movements of wrists, elbows and knee joints. This study provided a broad development potential for tough, transparent and conductive hydrogels as body-surface intelligent health monitoring systems and implantable soft electronics.
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Si, Liqi, Xiaowen Zheng, Jun Nie, Ruixue Yin, Yujie Hua, and Xiaoqun Zhu. "Silicone-based tough hydrogels with high resilience, fast self-recovery, and self-healing properties." Chemical Communications 52, no. 54 (2016): 8365–68. http://dx.doi.org/10.1039/c6cc02665f.

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A dual-component polymer hydrogel was prepared by one-pot, tandem polymerization. The concentration of monomer could be tuned freely due to the good water solubility of both monomers. The prepared hydrogels exhibited toughness, high resilience, fast self-recovery, and self-healing properties.
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Künzel, Matthias, and Marc in het Panhuis. "Strain sensors based on conducting poly(acrylamide) hydrogels." MRS Advances 5, no. 17 (2020): 917–25. http://dx.doi.org/10.1557/adv.2020.112.

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ABSTRACTA simple model system towards an impedance-probing strain sensor based on conducting tough hydrogels is demonstrated. A poly(acrylamide) hydrogel, cross-linked with N,N’-methylene-bis(acrylamide) was contacted with carbon fibres for electrical impedance analysis. The conductivity of the salt-containing hydrogel was determined to be 114 ± 10 mS/cm. Upon stretching the hydrogel samples to their fourfold initial length, the impedance response increased according to a power law. This was used to establish a sensing equation for the relation between the resistive component of the impedance signal and the applied mechanical strain under tension. This work contributes to the development of highly stretchable and soft strain sensors for applications in soft robotics.
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Wang, Jilong, Yan Liu, Siheng Su, et al. "Ultrasensitive Wearable Strain Sensors of 3D Printing Tough and Conductive Hydrogels." Polymers 11, no. 11 (2019): 1873. http://dx.doi.org/10.3390/polym11111873.

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In this study, tough and conductive hydrogels were printed by 3D printing method. The combination of thermo-responsive agar and ionic-responsive alginate can highly improve the shape fidelity. With addition of agar, ink viscosity was enhanced, further improving its rheological characteristics for a precise printing. After printing, the printed construct was cured via free radical polymerization, and alginate was crosslinked by calcium ions. Most importantly, with calcium crosslinking of alginate, mechanical properties of 3D printed hydrogels are greatly improved. Furthermore, these 3D printed hydrogels can serve as ionic conductors, because hydrogels contain large amounts of water that dissolve excess calcium ions. A wearable resistive strain sensor that can quickly and precisely detect human motions like finger bending was fabricated by a 3D printed hydrogel film. These results demonstrate that the conductive, transparent, and stretchable hydrogels are promising candidates as soft wearable electronics for healthcare, robotics and entertainment.
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Jiang, Haoyang, Lixia Fan, Shuang Yan, Feibo Li, Huanjun Li, and Jianguo Tang. "Tough and electro-responsive hydrogel actuators with bidirectional bending behavior." Nanoscale 11, no. 5 (2019): 2231–37. http://dx.doi.org/10.1039/c8nr07863g.

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31

Luo, Qiaomei, Yangyang Shan, Xia Zuo, and Jiaqi Liu. "Anisotropic tough poly(vinyl alcohol)/graphene oxide nanocomposite hydrogels for potential biomedical applications." RSC Advances 8, no. 24 (2018): 13284–91. http://dx.doi.org/10.1039/c8ra00340h.

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Du, Juan, Shimei Xu, Shun Feng, Lina Yu, Jide Wang, and Yumei Liu. "Tough dual nanocomposite hydrogels with inorganic hybrid crosslinking." Soft Matter 12, no. 6 (2016): 1649–54. http://dx.doi.org/10.1039/c5sm02790j.

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33

Ballance, William C., Vignesh Karthikeyan, Inkyu Oh, et al. "Preoperative vascular surgery model using a single polymer tough hydrogel with controllable elastic moduli." Soft Matter 16, no. 34 (2020): 8057–68. http://dx.doi.org/10.1039/d0sm00981d.

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34

Liu, Tao, Ripeng Zhang, Jianzhi Liu, Ling Zhao, and Yueqin Yu. "High strength and conductive hydrogel with fully interpenetrated structure from alginate and acrylamide." e-Polymers 21, no. 1 (2021): 391–97. http://dx.doi.org/10.1515/epoly-2021-0043.

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Abstract Highly stretched and conductive hydrogels, especially synthetized from natural polymers, are beneficial for highly stretched electronic equipment which is applied in extreme environment. We designed and prepared robust and tough alginate hydrogels (GMA-SA-PAM) using the ingenious strategy of fully interpenetrating cross-linking, in which the glycidyl methacrylate (GMA) was used to modify sodium alginate (SA) and then copolymerized with acrylamide (AM) and methylenebisacrylamide (BIS) as cross-linkers. The complete cross-linked structures can averagely dissipate energy and the polymer structures can maintain hydrogels that are three-dimensional to greatly improve the mechanical performance of hydrogels. The GMA-SA-PAM hydrogels display ultra-stretchable (strain up to ∼407% of tensile strain) and highly compressible (∼57% of compression strain) properties. In addition, soaking the GMA-SA-PAM hydrogel in 5 wt% NaCl solution also endows the conductivity of the hydrogel (this hydrogel was named as GSP-Na) with excellent conductive properties (5.26 S m−1). The GSP-Na hydrogel with high stability, durability, as well as wide range extent sensor is also demonstrated by researching the electrochemical signals and showing the potential for applications in wearable and quickly responded electronics.
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35

Jiang, Haoyang, Gongzheng Zhang, Feibo Li, et al. "A self-healable and tough nanocomposite hydrogel crosslinked by novel ultrasmall aluminum hydroxide nanoparticles." Nanoscale 9, no. 40 (2017): 15470–76. http://dx.doi.org/10.1039/c7nr04722c.

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36

Wang, Zhenwu, Yang Cong, and Jun Fu. "Stretchable and tough conductive hydrogels for flexible pressure and strain sensors." Journal of Materials Chemistry B 8, no. 16 (2020): 3437–59. http://dx.doi.org/10.1039/c9tb02570g.

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37

Jing, Xin, Heng Li, Hao-Yang Mi, et al. "A flexible semitransparent dual-electrode hydrogel based triboelectric nanogenerator with tough interfacial bonding and high energy output." Journal of Materials Chemistry C 8, no. 17 (2020): 5752–60. http://dx.doi.org/10.1039/c9tc06937b.

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38

Dou, Qingqing, Zhi Wei Kenny Low, Kangyi Zhang, and Xian Jun Loh. "A new light triggered approach to develop a micro porous tough hydrogel." RSC Advances 7, no. 44 (2017): 27449–53. http://dx.doi.org/10.1039/c7ra03214e.

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39

Park, Shiwha, Seth Edwards, Shujie Hou, Ryann Boudreau, Rachel Yee, and Kyung Jae Jeong. "A multi-interpenetrating network (IPN) hydrogel with gelatin and silk fibroin." Biomaterials Science 7, no. 4 (2019): 1276–80. http://dx.doi.org/10.1039/c8bm01532e.

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40

Yang, Tianyu, Mian Wang, Fei Jia, Xiuyan Ren, and Guanghui Gao. "Thermo-responsive shape memory sensors based on tough, remolding and anti-freezing hydrogels." Journal of Materials Chemistry C 8, no. 7 (2020): 2326–35. http://dx.doi.org/10.1039/c9tc05804d.

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41

Heidarian, Pejman, Abbas Z. Kouzani, Akif Kaynak, Ali Zolfagharian, and Hossein Yousefi. "Dynamic Mussel-Inspired Chitin Nanocomposite Hydrogels for Wearable Strain Sensors." Polymers 12, no. 6 (2020): 1416. http://dx.doi.org/10.3390/polym12061416.

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It is an ongoing challenge to fabricate an electroconductive and tough hydrogel with autonomous self-healing and self-recovery (SELF) for wearable strain sensors. Current electroconductive hydrogels often show a trade-off between static crosslinks for mechanical strength and dynamic crosslinks for SELF properties. In this work, a facile procedure was developed to synthesize a dynamic electroconductive hydrogel with excellent SELF and mechanical properties from starch/polyacrylic acid (St/PAA) by simply loading ferric ions (Fe3+) and tannic acid-coated chitin nanofibers (TA-ChNFs) into the hydrogel network. Based on our findings, the highest toughness was observed for the 1 wt.% TA-ChNF-reinforced hydrogel (1.43 MJ/m3), which is 10.5-fold higher than the unreinforced counterpart. Moreover, the 1 wt.% TA-ChNF-reinforced hydrogel showed the highest resistance against crack propagation and a 96.5% healing efficiency after 40 min. Therefore, it was chosen as the optimized hydrogel to pursue the remaining experiments. Due to its unique SELF performance, network stability, superior mechanical, and self-adhesiveness properties, this hydrogel demonstrates potential for applications in self-wearable strain sensors.
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42

Yin, Jianyu, Shenxin Pan, Lili Wu, et al. "A self-adhesive wearable strain sensor based on a highly stretchable, tough, self-healing and ultra-sensitive ionic hydrogel." Journal of Materials Chemistry C 8, no. 48 (2020): 17349–64. http://dx.doi.org/10.1039/d0tc04144k.

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43

Costa, Ana M. S., and João F. Mano. "Highly robust hydrogels via a fast, simple and cytocompatible dual crosslinking-based process." Chemical Communications 51, no. 86 (2015): 15673–76. http://dx.doi.org/10.1039/c5cc05564d.

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44

Xu, Jianyu, Ziwen Fan, Lijie Duan, and Guanghui Gao. "A tough, stretchable, and extensively sticky hydrogel driven by milk protein." Polymer Chemistry 9, no. 19 (2018): 2617–24. http://dx.doi.org/10.1039/c8py00319j.

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45

Son, Young Jun, Jin Woo Bae, Ho Jung Lee, et al. "Humidity-resistive, elastic, transparent ion gel and its use in a wearable, strain-sensing device." Journal of Materials Chemistry A 8, no. 12 (2020): 6013–21. http://dx.doi.org/10.1039/d0ta00090f.

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46

Yang, Yiming, Chao Wang, Clinton G. Wiener, et al. "Tough Stretchable Physically-Cross-linked Electrospun Hydrogel Fiber Mats." ACS Applied Materials & Interfaces 8, no. 35 (2016): 22774–79. http://dx.doi.org/10.1021/acsami.6b08255.

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Wang, Xiaohan, Yi Si, Kai Zheng, Xuhong Guo, Jie Wang, and Yisheng Xu. "Mussel-Inspired Tough Double Network Hydrogel As Transparent Adhesive." ACS Applied Polymer Materials 1, no. 11 (2019): 2998–3007. http://dx.doi.org/10.1021/acsapm.9b00698.

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48

Fu, Rumin, Lingjie Tu, Yahong Zhou, et al. "A Tough and Self-Powered Hydrogel for Artificial Skin." Chemistry of Materials 31, no. 23 (2019): 9850–60. http://dx.doi.org/10.1021/acs.chemmater.9b04041.

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49

Fan, Changjiang, Liqiong Liao, Chao Zhang, and Lijian Liu. "A tough double network hydrogel for cartilage tissue engineering." Journal of Materials Chemistry B 1, no. 34 (2013): 4251. http://dx.doi.org/10.1039/c3tb20600a.

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50

Liu, Xiao-jiu, Ye-min Zhang, and Xin-song Li. "Tough biopolymer IPN hydrogel fibers by bienzymatic crosslinking approach." Chinese Journal of Polymer Science 33, no. 12 (2015): 1741–49. http://dx.doi.org/10.1007/s10118-015-1717-9.

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