Reversibly Transforming a Highly Swollen Polyelectrolyte Hydrogel to an Extremely Tough One and its Application as a Tubular Grasper

Yu, Hongjun; Zheng, Si Yu; Fang, Lingtao; Ying, Zhimin; Du, Ming; Wang, Jing; Ren, Keke; Wu, Zi Liang; Zheng, Qiang

doi:10.1002/adma.202005171

Cited by 158 publications

(160 citation statements)

References 67 publications

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“…The structure and nature of carboxyl-containing monomer greatly affect the mechanical properties of the resultant hydrogels, as revealed by control experiments of the hydrogels prepared with identical compositions yet different monomers: i) the presence of hydrophobic methyl group on the carboxyl groups can further improve the strength of coordination bonds and thus the mechanical performances of the gels. [47] ii) Using monomer containing multiple carboxyl groups leads to increased density of metal-coordination bonds and thus favors improved mechanical properties of the gels.…”

Section: Universality To Toughen Hydrogels By Forming Carboxyl-zr 4+ Coordination Bondsmentioning

confidence: 99%

Engineering Tough Metallosupramolecular Hydrogel Films with Kirigami Structures for Compliant Soft Electronics

Hao

Zhang

et al. 2021

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A simple and effective approach is demonstrated to fabricate tough metallosupramolecular hydrogel films of poly(acrylic acid) by one‐pot photopolymerization of the precursor solution in the presence of Zr4+ ions that form coordination complexes with the carboxyl groups and serve as the physical crosslinks of the matrix. Both as‐prepared and equilibrated hydrogel films are transparent, tough, and stable over a wide range of temperature, ionic strength, and pH. The thickness of the films can be easily tailored with minimum value of ≈7 μm. Owing to the fast polymerization and gelation process, kirigami structures can be facilely encoded to the gel films by photolithographic polymerization, affording versatile functions such as additional stretchability and better compliance of the planar films to encapsulate objects with sophisticated geometries that are important for the design of soft electronics. By stencil printing of liquid metal on the hydrogel film with a kirigami structure, the integrated soft electronics shows good compliance to cover curved surfaces and high sensitivity to monitor human motions. Furthermore, this strategy is applied to diverse natural and synthetic macromolecules containing carboxyl groups to develop tough hydrogel films, which will open opportunities for the applications of hydrogel films in biomedical and engineering fields.

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Section: Universality To Toughen Hydrogels By Forming Carboxyl-zr 4+ Coordination Bondsmentioning

confidence: 99%

Engineering Tough Metallosupramolecular Hydrogel Films with Kirigami Structures for Compliant Soft Electronics

Hao

Zhang

et al. 2021

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“…Taking advantage of the DN principle, non‐covalent bonds (e.g., ionic bond, hydrogen bond, and metal–ligand bond) have also been introduced into hydrogel networks as reversible sacrificial bonds, endowing self‐healing properties. [ 22–27 ] By introducing calcium ions (Ca 2+ ) into the first network to form metal–ligand bonds, Suo and coworkers have developed tough and recoverable DN gels, while possessing relatively low strength. [ 28 ] Instead of the DN strategy, we have also achieved strong and tough dually cross‐linked poly(acrylic acid) (PAAc) hydrogels via a saline solution soaking method.…”

Section: Introductionmentioning

confidence: 99%

Strong Tough Polyampholyte Hydrogels via the Synergistic Effect of Ionic and Metal–Ligand Bonds

Huang

Xiao

Zhou

et al. 2021

Adv Funct Materials

123

126

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Despite existing in biological systems, developing synthetic polyampholyte (PA) hydrogels constructed by both ionic and metal–ligand bonds remains challenging. Herein, a simple secondary equilibrium approach is proposed to fabricate strong and tough PA hydrogels via the synergy of ionic and metal–ligand bonds. The original PA gels (constructed by ionic bonds) are first dialyzed in multivalent metal‐ion solutions to reach a swelling equilibrium and then moved to deionized water to dialyze excess free ions to achieve a new equilibrium. Through this approach, the original PA gel network can be optimized and eventually constructed by ionic and metal–ligand bonds, enabling a synergistic reinforcement. By selecting different original PA gel systems and diverse multivalent metal‐ions, the proposed approach is proved to be generalizable to fabricate strong and tough PA gels. Additionally, the hydrogels have stable ion‐conductivity even at the water‐equilibrium state, making them promising as strain sensors. The viscoelastic and elastic contributions to the mechanical properties of the hydrogels by a viscoelastic model are also discussed to further understand the strengthening and toughening mechanisms. The proposed strategy is simple but effective for achieving strong and tough PA‐based hydrogels. This study also provides new insights for PA hydrogels in electrolyte environments.

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“…[ 120 ] The stretching‐induced linearly oriented PBDT was crosslinked and fixed in ZrCl 2 O solution to produce a strengthened and stiffened DN gel. Because an octavalent tetramer complex [Zr(OH) 2 ·4H 2 O] 4 8+ is generated in the ZrCl 2 O solution and the PBDT sulfonate groups consequently form a [Zr(OH) 2 ·4H 2 O] 4 8+ –PBDT coordination complex, [ 135–137 ] the stretched PBDT chains can be fixed due to the formation of strong bonding by the octavalent Zr cluster. As a result, the tensile strength and elastic modulus increased by 1.8 times from 1.2 to 2.2 MPa and by 1.3 times from 1.0 to 1.3 MPa, respectively (Figure 7f, dark green and dark brown lines).…”

Section: Polymer Matrix Manipulation By Aligning Polymer Chainsmentioning

confidence: 99%

Recent Strategies for Strengthening and Stiffening Tough Hydrogels

Kim

2021

Advanced NanoBiomed Research

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Hydrogels are major components of the human body. To replace a damaged hydrogel in the body or support/monitor its normal operation, artificial hydrogels similar to those found in nature are required. As the development of morphologically adaptable soft yet tough hydrogels such as double‐network (DN) and polyampholyte (PA) gels, they are applied to soft tissues such as the neural and epithelial tissues with elastic moduli ranging from a few pascals to several kilopascals. However, creating strong and stiff hydrogels emulating stiff load‐bearing connective tissues with elastic moduli in the MPa‐to‐GPa range remains challenging. Herein, recent strategies and potential methods for strengthening and stiffening tough DN and PA gels (such as the reinforcement addition, polymer chain alignment, and solvent exchange) as well as the reinforcing and fracture mechanisms of the resulting hydrogels are summarized. The objective is to provide some insights into the optimal strategy and method for fabricating hydrogels with a combination of strength, stiffness, and toughness, which can emulate natural load‐bearing tissues.

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Reversibly Transforming a Highly Swollen Polyelectrolyte Hydrogel to an Extremely Tough One and its Application as a Tubular Grasper

Abstract: Polyelectrolyte (PE) hydrogels are typical soft materials with extremely high swelling capacity due to the high osmotic pressure of the dissociated counterions. [1] For example,

Cited by 158 publications

References 67 publications

Engineering Tough Metallosupramolecular Hydrogel Films with Kirigami Structures for Compliant Soft Electronics

Engineering Tough Metallosupramolecular Hydrogel Films with Kirigami Structures for Compliant Soft Electronics

Strong Tough Polyampholyte Hydrogels via the Synergistic Effect of Ionic and Metal–Ligand Bonds

Recent Strategies for Strengthening and Stiffening Tough Hydrogels

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