Highly Stretchable and Instantly Recoverable Slide-Ring Gels Consisting of Enzymatically Synthesized Polyrotaxane with Low Host Coverage

Jiang, Lan Ying; Liu, Chang; Mayumi, Koichi; Katō, K.; Yokoyama, Haruki; Ito, Kohzo

doi:10.1021/acs.chemmater.8b01208

Cited by 152 publications

(155 citation statements)

References 41 publications

(63 reference statements)

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“…In previous reports, Young’s modulus in slide-ring gels showed a similar value regardless of the number of threaded cyclic molecules in PRXs, although Young’s modulus increased with a higher cross-linking density [24,41]. In the present study, at the 1% strain point, Young’s modulus was controlled by the amount of EDC/NHS regardless of the type of cross-linker used (Table 2).…”

Section: Resultssupporting

confidence: 72%

“…Slide-ring gels synthesized by the chemical cross-linking of PRXs show distinct properties from those of conventional physical and chemical hydrogels [22,23]. The cross-linking points in the slide-ring gels can be freely shifted by the movable α-CDs in PRXs along with an axle polymer [24]. When the slide-ring gels are deformed, the stress applied to hydrogels can be dispersed by movement of the cross-linking points without bond breaking, which leads to unique mechanical properties such as high stretchability and toughness [25,26].…”

Section: Introductionmentioning

confidence: 99%

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Mechanically Reinforced Gelatin Hydrogels by Introducing Slidable Supramolecular Cross-Linkers

et al. 2019

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Tough mechanical properties are generally required for tissue substitutes used in regeneration of damaged tissue, as these substitutes must be able to withstand the external physical force caused by stretching. Gelatin, a biopolymer derived from collagen, is a biocompatible and cell adhesive material, and is thus widely utilized as a component of biomaterials. However, the application of gelatin hydrogels as a tissue substitute is limited owing to their insufficient mechanical properties. Chemical cross-linking is a promising method to improve the mechanical properties of hydrogels. We examined the potential of the chemical cross-linking of gelatin hydrogels with carboxy-group-modified polyrotaxanes (PRXs), a supramolecular polymer comprising a poly(ethylene glycol) chain threaded into the cavity of α-cyclodextrins (α-CDs), to improve mechanical properties such as stretchability and toughness. Cross-linking gelatin hydrogels with threading α-CDs in PRXs could allow for freely mobile cross-linking points to potentially improve the mechanical properties. Indeed, the stretchability and toughness of gelatin hydrogels cross-linked with PRXs were slightly higher than those of the hydrogels with the conventional chemical cross-linkers 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide (EDC)/N-hydroxysuccinimide (NHS). In addition, the hysteresis loss of gelatin hydrogels cross-linked with PRXs after repeated stretching and relaxation cycles in a hydrated state was remarkably improved in comparison with that of conventional cross-linked hydrogels. It is considered that the freely mobile cross-linking points of gelatin hydrogels cross-linked with PRXs attenuates the stress concentration. Accordingly, gelatin hydrogels cross-linked with PRXs would provide excellent mechanical properties as biocompatible tissue substitutes exposed to a continuous external physical force.

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Section: Resultssupporting

confidence: 72%

Section: Introductionmentioning

confidence: 99%

Mechanically Reinforced Gelatin Hydrogels by Introducing Slidable Supramolecular Cross-Linkers

et al. 2019

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“…Recently, the slide‐ring gel, composed of a polyrotaxane cross‐linked polymer network with high content of solvent, [6] has been widely regarded as a type of highly elastic chemically cross‐linked gel, where the “ring” linked to the polymer chain can slide freely through the axis, giving the gel network excellent internal stress dispersion ability [7] . However, similar to the case of the double‐network gel, the synthesis of slide‐ring hydrogels is exceedingly difficult, mainly because of the low synthesis efficiency of the polyrotaxane.…”

Section: Methodsmentioning

confidence: 99%

Highly Elastic Slide‐Ring Hydrogel with Good Recovery as Stretchable Supercapacitor

Jia

Chen

et al. 2020

Chemistry A European J

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As a new material with excellent mechanical properties and good stability, slide‐ring gels have attracted attention and research. However, they cannot be widely used due to their relatively complicated synthesis. Herein, we use 6‐acrylamidomethylether‐modified α‐cyclodextrin (αCDAAmMe) and PEG20000 diacrylate (PEG20000DA) to construct a polypseudorotaxane. Then, the polypseudorotaxane reacts with acrylamide via a photo‐initiated polymerization in situ to conveniently obtain a slide‐ring hydrogel with good elastic property and high recovery property. The hydrogel can be easily stretched to 22.5 times of its original length but recovered rapidly and almost reversibly. These results enable the application of hydrogel to make an intrinsically stretchable and compressible supercapacitor after doping ions and the adhesion of commercially available carbon nanotube (CNT) paper as electrodes, giving the ionic conductivity of 17.0 mS cm−1 (comparable to that of the commercial PVA/H3PO4 electrolyte) and the capacitance of 0.87 μF cm−2 (at the scan speed of 100 mV s−1), and its capacitance can be further enhanced under stretching.

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“…Mechanically induced conformational change in molecules falls within so-called mechanochemistry, whose main principle is the Karino et al, 2006;Mayumi et al, 2012;Kato et al, 2013Kato et al, , 2015Noda et al, 2014;Liu et al, 2017;Jiang et al, 2018 Liquid crystal elastomers (LCEs)…”

Section: Polymers With Conformational Instabilitiesmentioning

confidence: 99%

“…This capability, from a mechanical standpoint, makes it possible to avoid the stress concentration taking place in the shortest chains-as typically occurs in standard polymers-that more easily reach their maximum extension (related to the number of Kuhn's segments per chain N and their length b as λ max = b √ N) and consequently fail. On the other hand, when the network possesses movable ring connections, the polymer chains can freely move through the cross-link sites, allowing the tension induced by external stress to be evenly distributed throughout the whole material (Kato et al, 2013;Jiang et al, 2018). From the mechanical viewpoint, the crosslink sites behave as a pulley, and thus the cooperative work is referred to as a pulley effect.…”

Section: Slide-ring Gels: a Topological Gel With Slidable Cross-linksmentioning

confidence: 99%

Smart Polymers for Advanced Applications: A Mechanical Perspective Review

2020

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Responsive materials, as well as active structural systems, are today widely used to develop unprecedented smart devices, sensors, or actuators; their functionalities come from the ability to respond to environmental stimuli with a detectable reaction. Depending on the responsive material under study, the triggering stimuli can have a different nature, ranging from physical (temperature, light, electric or magnetic field, mechanical stress, etc.), chemical (pH, ligands, etc.), or biological (enzymes, etc.) type. Such a responsiveness can be obtained by properly designing the meso-or macroscopic arrangement of the constitutive elements, as occurs in metamaterials, or can be obtained by using responsive materials per se, whose responsiveness comes from the chemistry underlying their microstructure. In fact, when the responsiveness at the molecular level is properly organized, the nanoscale response can be collectively detected at the macroscale, leading to a responsive material. In the present article, we review the enormous world of responsive polymers, by outlining the main features, characteristics, and responsive mechanisms of smart polymers and by providing a mechanical modeling perspective, both at the molecular as well as at the continuum scale level. We aim at providing a comprehensive overview of the main features and modeling aspects of the most diffused smart polymers. The quantitative mechanical description of active materials plays a key role in their development and use, enabling the design of advanced devices as well as to engineer the materials' microstructure according to the desired functionality.

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Highly Stretchable and Instantly Recoverable Slide-Ring Gels Consisting of Enzymatically Synthesized Polyrotaxane with Low Host Coverage

Cited by 152 publications

References 41 publications

Mechanically Reinforced Gelatin Hydrogels by Introducing Slidable Supramolecular Cross-Linkers

Mechanically Reinforced Gelatin Hydrogels by Introducing Slidable Supramolecular Cross-Linkers

Highly Elastic Slide‐Ring Hydrogel with Good Recovery as Stretchable Supercapacitor

Smart Polymers for Advanced Applications: A Mechanical Perspective Review

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