Extra‐Large Mechanical Anisotropy of a Hydrogel with Maximized Electrostatic Repulsion between Cofacially Aligned 2D Electrolytes

Sano, Koki; Arazoe, Yuka Onuma; Ishida, Yasuhiro; Ebina, Yasuo; Osada, Minoru; Sasaki, Takayoshi; Hikima, Takaaki; Aida, Takuzo

doi:10.1002/anie.201807240

Cited by 31 publications

(27 citation statements)

References 62 publications

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“…1a and Supplementary Fig. 1) [27][28][29][30] . TiNS is densely populated with negative charges (1.5 C m -2 ) that are surrounded by tetrabutylammonium countercations.…”

Section: Resultsmentioning

confidence: 99%

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A mechanically adaptive hydrogel with a reconfigurable network consisting entirely of inorganic nanosheets and water

et al. 2020

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Although various biomimetic soft materials that display structural hierarchies and stimuli responsiveness have been developed from organic materials, the creation of their counterparts consisting entirely of inorganic materials presents an attractive challenge, as the properties of such materials generally differ from those of living organisms. Here, we have developed a hydrogel consisting of inorganic nanosheets (14 wt%) and water (86 wt%) that undergoes thermally induced reversible and abrupt changes in its internal structure and mechanical elasticity (23-fold). At room temperature, the nanosheets in water electrostatically repel one another and self-assemble into a long-periodic lamellar architecture with mutually restricted mobility, forming a physical hydrogel. Upon heating above 55 °C, the electrostatic repulsion is overcome by competing van der Waals attraction, and the nanosheets rearrange into an interconnected 3D network of another hydrogel. By doping the gel with a photothermal-conversion agent, the gel-to-gel transition becomes operable spatiotemporally on photoirradiation.

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“…1a and Supplementary Fig. 1) [27][28][29][30] . TiNS is densely populated with negative charges (1.5 C m -2 ) that are surrounded by tetrabutylammonium countercations.…”

Section: Resultsmentioning

confidence: 99%

“…In this work, by adopting the above strategy, we succeeded in developing a stimuli-responsive hydrogel consisting of anionic nanosheets of titanate [27][28][29][30] (TiNSs; 14 wt%) and water (86 wt%) that, depending on the temperature, can reversibly adopt one of two hydrogel states: a repulsion-dominant state or an attractiondominant state (Fig. 1).…”

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confidence: 99%

A mechanically adaptive hydrogel with a reconfigurable network consisting entirely of inorganic nanosheets and water

et al. 2020

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“…A typical change is hydrogelation, which enables the design of attractive biomaterials, including cell culture scaffolds. Conventionally, the effects of cross-linking have been investigated using covalent polymers [ 68 , 69 , 70 , 71 , 72 , 73 , 74 , 75 , 76 , 77 , 78 ]. Mechanically robust nanocomposite hydrogels can be prepared by the use of clay nanosheets at cross-linking points [ 68 , 69 ].…”

Section: Effects Of Cross-linkingmentioning

confidence: 99%

“…For example, nanocomposite hydrogels with high water content and mechanical strength were formed by employing interactions between dendritic macromolecules having multiple guanidinium ions and clay nanosheets [ 69 ]. Hydrogels with mechanical anisotropy were also formed by replacing clay nanosheets with magnetically alignable titanate nanosheets [ 70 , 71 , 72 ]. Double network hydrogels embedding two different types of polymer networks give hydrogels with enhanced mechanical strengths [ 73 , 74 ].…”

Section: Effects Of Cross-linkingmentioning

confidence: 99%

“…A representative example is hydrogelation, which converts peptide fiber dispersions into self-standing materials for biomaterial applications including cell culture scaffolds. Cross-linking methods, which have been extensively developed using covalent water-soluble polymers [ 68 , 69 , 70 , 71 , 72 , 73 , 74 , 75 , 76 , 77 , 78 ], are also effective in the cases of supramolecular peptide fibers. In particular, unique cross-linking methods can be employed by taking advantage of the functionalities of amino acid residues in peptide fibers [ 79 , 80 , 81 , 82 , 83 , 84 , 85 , 86 , 87 , 88 , 89 , 90 ].…”

Section: Introductionmentioning

confidence: 99%

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Current Progress in Cross-Linked Peptide Self-Assemblies

Uchida

Muraoka

2020

IJMS

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Peptide-based fibrous supramolecular assemblies represent an emerging class of biomaterials that can realize various bioactivities and structures. Recently, a variety of peptide fibers with attractive functions have been designed together with the discovery of many peptide-based self-assembly units. Cross-linking of the peptide fibers is a key strategy to improve the functions of these materials. The cross-linking of peptide fibers forming three-dimensional networks in a dispersion can lead to changes in physical and chemical properties. Hydrogelation is a typical change caused by cross-linking, which makes it applicable to biomaterials such as cell scaffold materials. Cross-linking methods, which have been conventionally developed using water-soluble covalent polymers, are also useful in supramolecular peptide fibers. In the case of peptide fibers, unique cross-linking strategies can be designed by taking advantage of the functions of amino acids. This review focuses on the current progress in the design of cross-linked peptide fibers and their applications.

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Anisotropic Hybrid Hydrogels Constructed via the Noncovalent Assembly for Biomimetic Tissue Scaffold

Lin

Xing

et al. 2022

Adv Funct Materials

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Anisotropic structure is key for exploring the biomimetic functions of anisotropic hydrogels. However, the anisotropic hydrogel study should not be limited to its architecture design but must include the understanding and improvement of the internal interaction among their components. Herein, a noncovalent mediated assembly strategy is proposed to simultaneously improve the chitin chain mobility and enhance the interfacial interaction, for achieving anisotropic chitin/2D material (molybdenum disulfide and brushite as example) hydrogels via mechanical deformation. Tannic acid (TA) is used to i) introduce the dynamic noncovalent crosslinking structure among the chitin chains for affording considerable molecular mobility to allow chitin chains alignment under mechanical deformation; ii) enhance chitin–2D interfacial interaction for benefiting 2D materials orientation under the chitin chains driving. The design concept achieves multiple noncovalent assembly crosslinks (chitin–chitin, chitin–TA, and chitin–TA–2D) and biomimetic anisotropic nanofibrous morphology, leading to the superior mechanical performance. The anisotropic chitin–TA/brushite hydrogel effectively accelerates bone regeneration by promoting cell osteogenic differentiation and directional migration, showing potential in tissue engineering. It is anticipated that the noncovalent mediated assembly concept could be used to fabricate other polymer based composite anisotropic hydrogels for diverse applications.

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Extra‐Large Mechanical Anisotropy of a Hydrogel with Maximized Electrostatic Repulsion between Cofacially Aligned 2D Electrolytes

Cited by 31 publications

References 62 publications

A mechanically adaptive hydrogel with a reconfigurable network consisting entirely of inorganic nanosheets and water

A mechanically adaptive hydrogel with a reconfigurable network consisting entirely of inorganic nanosheets and water

Current Progress in Cross-Linked Peptide Self-Assemblies

Anisotropic Hybrid Hydrogels Constructed via the Noncovalent Assembly for Biomimetic Tissue Scaffold

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