A Dual‐Crosslinked Strategy to Construct Physical Hydrogels with High Strength, Toughness, Good Mechanical Recoverability, and Shape‐Memory Ability

Qin, Zhihui; Niu, Rui; Tang, Chenjue; Xia, Jun; Feng, Ji; Dong, Dianyu; Zhang, Haitao; Zhang, Shuo; Li, Junjie; Yao, Fanglian

doi:10.1002/mame.201700396

Cited by 62 publications

(49 citation statements)

References 56 publications

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“…In Figure S6, Supporting Information, the formation of network structure of the hydrogels was verified by FTIR. The characteristic bands at 1700–1600 cm −1 were attributed to –COO − stretching vibration, we can intuitively see that the p‐gel has a certain shift in the characteristic peak after soaking in Fe 3+ . This may be due to the formation of ion complexes between the –COO − and Fe 3+ to produce iron carboxylate complexes.…”

Section: Methodsmentioning

confidence: 75%

Integrated Functional High‐Strength Hydrogels with Metal‐Coordination Complexes and H‐Bonding Dual Physically Cross‐linked Networks

Liu

et al. 2018

Macromol. Rapid Commun.

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With the deepening of research on high-strength hydrogels, the multi-functional study of hydrogels has become a hot spot. In this paper, a dual cross-linked physical high-strength hydrogels is prepared by a relatively simple method. 2-Vinyl- 4,6-Diamino-2-vinyl-1,3,5-triazine (VDT) induces the formation of the first cross-linking points through the interaction of hydrogen bonds with poly(acrylamide-co-acrylic acid) (PAm-co-Ac) chains, then the secondary physical cross-linkers Fe that introduce ionic coordinates between Fe and -COO groups. Due to the synergistic effect of hydrogen bonding and ionic coordination, hydrogels possess high tensile strength (approx. 4.34 MPa), large elongation (approx. 17.64 times), and good healing properties under alkali solution after cutting into two pieces. Meanwhile, VDT contains diaminotriazine functional groups that easily form hydrogen bonds so that the polymer of hydrogels could absorb 5-fluorouridine. In addition, the contribution of ionic polymer segments enables pH to be sensitive to hydrogels and facilitates the adsorption of a large number of ionic monomers to form ionic conductive networks, the prepared hydrogel capacitor device has very high sensitivity to pressure and deformation, and can detect the movement behavior of the human body. The dual-physical cross-linked hydrogels had a selective adsorption to biological small molecules and could be assembled into a flexible wearable device with high sensitivity.

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Section: Methodsmentioning

confidence: 75%

Integrated Functional High‐Strength Hydrogels with Metal‐Coordination Complexes and H‐Bonding Dual Physically Cross‐linked Networks

Liu

et al. 2018

Macromol. Rapid Commun.

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“…Therefore, improving mechanical properties of hydrogels became an important research hotspot. So far, versatile strategies to achieve tough hydrogels have been emerged, including double-network hydrogels (Gong et al, 2003;Gong, 2014;Liang et al, 2016;Chen et al, 2018;Jing et al, 2019), nanocomposite hydrogels (Haraguchi and Takehisa, 2002;Chen et al, 2015;GhavamiNejad et al, 2016;Zhu et al, 2017), topological hydrogels (Okumura and Ito, 2001;Li et al, 2018), macromolecular microsphere composite hydrogels (Huang et al, 2007;Gu et al, 2016;Zhang and Khademhosseini, 2017;Wang Z. et al, 2018), hydrophobic association hydrogels (Li et al, 2012;Mihajlovic et al, 2017;Han et al, 2018), hydrogen bonding/dipole-dipole reinforced hydrogels (Han et al, 2012;Zhang et al, 2015;Qin et al, 2018), and many others (Gong et al, 2016;Liu J. et al, 2017;Zhao et al, 2019). However, almost all of the hydrogels swollen a large amount of water in polymer networks cannot resist a cold or hot environment (Wei et al, 2014(Wei et al, , 2015Wang W. et al, 2018), hindering the application of tough hydrogels in harsh conditions.…”

Section: Introductionmentioning

confidence: 99%

Physical Organohydrogels With Extreme Strength and Temperature Tolerance

et al. 2020

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Tough gel with extreme temperature tolerance is a class of soft materials having potential applications in the specific fields that require excellent integrated properties under subzero temperature. Herein, physically crosslinked Europium (Eu)-alginate/polyvinyl alcohol (PVA) organohydrogels that do not freeze at far below 0 • C, while retention of high stress and stretchability is demonstrated. These organohydrogels are synthesized through displacement of water swollen in polymer networks of hydrogel to cryoprotectants (e.g., ethylene glycol, glycerol, and d-sorbitol). The organohydrogels swollen water-cryoprotectant binary systems can be recovered to their original shapes when be bent, folded and even twisted after being cooled down to a temperature as low as −20 and −45 • C, due to lower vapor pressure and ice-inhibition of cryoprotectants. The physical organohydrogels exhibit the maximum stress (5.62 ± 0.41 MPa) and strain (7.63 ± 0.02), which is about 10 and 2 times of their original hydrogel, due to the synergistic effect of multiple hydrogen bonds, coordination bonds and dense polymer networks. Based on these features, such physically crosslinked organohydrogels with extreme toughness and wide temperature tolerance is a promising soft material expanding the applications of gels in more specific and harsh conditions.

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“…This could be due to that while the high MA content enhances hydrophobic association to promote tensile stress [Fig. (b1)], hydrophobic association could not recover a short time of 10 min due to a long relaxation time [Fig. (b2)].…”

Section: Results and Discussmentioning

confidence: 99%

Mechanically tough and recoverable hydrogels via dual physical crosslinkings

Yang

Ren

Cai

et al. 2018

J Polym Sci B Polym Phys

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Development of functional tough hydrogels with new network structures and energy dissipation mechanisms has great promise for many applications. Here, a new type of physical hydrogel crosslinked by hydrophobic association and hydrogen bonds was synthesized by a facile micellar copolymerization of hydrophobic methyl acrylate (MA) monomers and hydrophilic N-hydroxyethyl acrylamide (HEAA) monomers in the presence of Tween80 micelles. Strong hydrophobic association between inner MA and Tween80 and hydrogen bonds between external polyHEAA and Tween80 provide two distinct crosslinkers to construct mechanically tough and recoverable network. Mechanical properties of polyHEAA-MA@Tween80 hydrogels strongly depended on network components (HEAA, MA; Tween80 concentrations). At optimal conditions, the hydrogels can achieve fracture stress of 700 kPa, fracture strain of 1687 mm/mm, elastic modulus of 195 kPa, and tearing energy of 1598 J/m 2 . Due to the reversible nature of physical interactions, polyHEAA-MA@Tween80 hydrogels can achieve fast stiffness/toughness recovery of 60%/33% without any external stimuli and resting time at room temperature. This work demonstrates a new design strategy to fabricate a new a singlenetwork hydrogel with high mechanical and self-recovery properties by incorporating both hydrophobic association and hydrogen bonds in the network, which may provide alternative viewpoint for the design of multifunctional tough hydrogels.

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A Dual‐Crosslinked Strategy to Construct Physical Hydrogels with High Strength, Toughness, Good Mechanical Recoverability, and Shape‐Memory Ability

Cited by 62 publications

References 56 publications

Integrated Functional High‐Strength Hydrogels with Metal‐Coordination Complexes and H‐Bonding Dual Physically Cross‐linked Networks

Integrated Functional High‐Strength Hydrogels with Metal‐Coordination Complexes and H‐Bonding Dual Physically Cross‐linked Networks

Physical Organohydrogels With Extreme Strength and Temperature Tolerance

Mechanically tough and recoverable hydrogels via dual physical crosslinkings

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