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1.
Kwanchai Buaksuntear Phakamat Limarun Supitta Suethao Wirasak Smitthipong 《International journal of molecular sciences》2022,23(13)
Supramolecular polymers are widely utilized and applied in self-assembly or self-healing materials, which can be repaired when damaged. Normally, the healing process is classified into two types, including extrinsic and intrinsic self-healable materials. Therefore, the aim of this work is to review the intrinsic self-healing strategy based on supramolecular interaction or non-covalent interaction and molecular recognition to obtain the improvement of mechanical properties. In this review, we introduce the main background of non-covalent interaction, which consists of the metal–ligand coordination, hydrogen bonding, π–π interaction, electrostatic interaction, dipole–dipole interaction, and host–guest interactions, respectively. From the perspective of mechanical properties, these interactions act as transient crosslinking points to both prevent and repair the broken polymer chains. For material utilization in terms of self-healing products, this knowledge can be applied and developed to increase the lifetime of the products, causing rapid healing and reducing accidents and maintenance costs. Therefore, the self-healing materials using supramolecular polymers or non-covalent interaction provides a novel strategy to enhance the mechanical properties of materials causing the extended cycling lifetime of products before replacement with a new one. 相似文献
2.
Shear-thinning and self-healing hydrogels are being investigated in various biomedical applications including drug delivery, tissue engineering, and 3D bioprinting. Such hydrogels are formed through dynamic and reversible interactions between polymers or polypeptides that allow these shear-thinning and self-healing properties, including physical associations (e.g., hydrogen bonds, guest–host interactions, biorecognition motifs, hydrophobicity, electrostatics, and metal–ligand coordination) and dynamic covalent chemistry (e.g., Schiff base, oxime chemistry, disulfide bonds, and reversible Diels–Alder). Their shear-thinning properties allow for injectability, as the hydrogel exhibits viscous flow under shear, and their self-healing nature allows for stabilization when shear is removed. Hydrogels can be formulated as uniform polymer and polypeptide assemblies, as hydrogel nanocomposites, or in granular hydrogel form. This review focuses on recent advances in shear-thinning and self-healing hydrogels that are promising for biomedical applications. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48668. 相似文献
3.
Responsive hydrogels hold great promise for applications such as biological tissue engineering, controlled drug release, soft actuators, and intelligent sensors. However, the design and construction of robust responsive hydrogels using a simple method remains a significant challenge. Herein, a non-covalently crosslinked responsive hydrogel was constructed by introducing carboxyl-Zr4+ metal coordination to the hydrophobic association network of P(AA-co-LMA) hydrogel through a facile one-pot polymerization method. The incorporation of multiple reversible interactions, including hydrogen bonding, metal coordination, and hydrophobic association, resulted in a responsive hydrogel with exceptional mechanical strength (≈2.92 MPa), outstanding flexibility (elongation>1000%), and rapid response to pH alterations. Furthermore, the hydrogel also presented good ionic conductivity due to the abundant movable ions, as well as high sensitivity and stability. As application demonstrations, the supermolecular hydrogel had been successfully used in actuating and strain sensing. This work establishes an effective design strategy for creating tough and multifunctional responsive hydrogel. 相似文献
4.
Hydrogels are attractive materials for constructing underwater antifouling coatings on solid substrates. However, the application of hydrogel coatings usually faces the obstacles of complex preparation process and poor durability. Herein, we present a facile method to prepare durable hydrogel coatings on metal foils based on rationally designed supramolecular polyurea (PU) hydrogels. PU hydrogels are designed to be cross-linked with hydrogen bonds (H-bonds) and hydrophobic interactions in the hard segment domains by using dihydrazides with different alkyl spacer lengths ( (CH2)m ) as chain extender. The synergy of H-bond and hydrophobic interaction can stabilize H-bonds in water, as confirmed by Raman spectroscopy. As a result, PU hydrogels exhibit antiswelling capacity and robustness in both deionized water and seawater. Subsequently, PU hydrogel coatings on Cu/Al foils are prepared by convenient brush coating and subsequent swelling. The resulting hydrogel coatings exhibit excellent underwater anti-oil-adhesion and self-cleaning property, and are durable enough to withstand various static and dynamic damaging tests. The good durability of PU hydrogel coatings should be ascribed to the robust adhesion interface and excellent antiswelling capacity of PU hydrogels. The combination of facile preparation and good durability makes PU hydrogel coatings promising candidates for reliable underwater antifouling. 相似文献
5.
Physically Linked PVA/P(AAm‐co‐SMA) Hydrogels: Tough,Fast Recovery,Antifatigue, and Self‐Healing Soft Materials
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Wen Jiang Zheng Yang Gao Xiao Xi Fan Xiao Feng Cui Wei Zou Dan Zheng Jie Yan Bin Li 《大分子材料与工程》2018,303(7)
The application of traditional chemically crosslinked hydrogels is often limited by poor mechanical properties because of their own inhomogeneous network and irreversible crosslinking bonds. Herein, physical interactions are applied to crosslink the interpenetrating network hydrogel, i.e., hydrogen bonding and crystalline domain for polyvinyl alcohol network, and hydrophobic interaction inside micelle for poly (acrylamide‐co‐stearyl methyl acrylate) [P(AAm‐co‐SMA)] network. In this gel network system, reversible energy dissipation mechanism is realized by dissociation and reassociation of weak interactions including hydrogen bonding and hydrophobic interaction inside the micelle. Strong crystalline domains serve as permanent crosslinking interactions to maintain network integrity under large extension. As a result, the synergy of weak and strong interactions leads to tough, antifatigue, fast recovery, and self‐healing properties of the hydrogel. This proposed strategy of achieving versatile hydrogels can broaden the use of hydrogels into load‐bearing applications. 相似文献
6.
Polypseudorotaxane (PPR) hydrogels formed by inclusion complexes between poly(ethylene glycol) (PEG) and α-cyclodextrin (α-CD) are highlighted as promising biomaterial for drug delivery. Here, we report a novel injectable PPR hydrogel containing graphene oxide (GO) for pH-responsive controlled release of doxorubicin hydrochloride (DOX). Our results showed that the gelation rates of the PEG/α-CD supramolecular structures could be tailored depending on the reagent concentrations. The formation of PEG/α-CD inclusion complexes was confirmed by TEM and XRD, the latter further confirming that GO restricts their formation. The supramolecular hydrogels were easily loaded with DOX by simple addition into the PEG solution before the complex formation with the α-CD solution. Noteworthy, disruption of ionic interactions between DOX and GO in the nanocomposite at pH = 5.5 resulted in higher DOX release than under physiological conditions (pH = 7.4). This pH dependence was barely observed in pure PPR hydrogel. These findings introduce DOX-loaded supramolecular hydrogels nanocomposites as promising carriers for pH-responsive and therefore localized, drug delivery systems. 相似文献
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8.
Umit Gulyuz 《大分子材料与工程》2021,306(9):2100201
Herein, a series of poly(methacrylic acid) hydrogels are prepared via bulk polymerization of methacrylic acid (MAAc) and grafting of Triton X-100 (TX-100). One-pot and extremely simple chemistry consist of only mixing and subsequently heating of commercially available monomer and surfactant. The polymer chains are interconnected through dual physical cross-link points formed by the hydrophobic associations in the center of TX-100 micelles and hydrogen bonds stabilized by hydrophobic α-methyl groups of MAAc. The hydrogels exhibit tunable mechanical properties ranging between softness and stiffness by adjusting the surfactant/monomer molar ratio, such as Young modulus of 0.6−22 MPa, elongation at break of 750−1700%, tensile strength of 0.21−3.6 MPa, and compressive strength of 41−93 MPa. The synergistic effect of high-density hydrogen bonds with hydrophobic associations endows a plastic-like hydrogel with high strength and shape memory (SM) behavior, while a high concentration of micelles with low-density hydrogen bonds endows a stretchable elastic hydrogel. The combination of temperature-induced SM property and wide-ranging mechanical performance will make such hydrogels useful in diverse applications. 相似文献
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10.
Mehrnoosh Hasan Shahriari Majid Abdouss Afra Hadjizadeh 《Polymer Engineering and Science》2023,63(3):798-810
Hydrogels have the potential to simulate and permeate body tissues. They can be used in many biomedical applications, such as drug delivery, wound dressings, contact lenses, synthetic implants, biosensors, and tissue engineering. Despite recent significant advances in hydrogel fabrication, with the introduction of double network hydrogels, with ionic or hydrogen bonds, there is still the challenge of achieving optimal mechanical properties with appropriate self-healing ability. To solve the above problem, in this study, a new type of starch/chitosan/PVA/borax hydrogel was synthesized by adopting the one-pot method. The effect of concentration and ratio of raw materials on the final properties of hydrogels, such as the degree of hydrophilicity, morphology, degradation, mechanical strength, and drug release rate, was investigated. The properties of hydrogels were examined by scanning electron microscopy, thermogravimetric analysis, Fourier-transform infrared spectroscopy, X-ray diffractometry, and contact angle, which confirmed the composite synthesis and uniform distribution of HNT and curcumin. In addition, the composite hydrogel showed excellent mechanical properties. Drug release studies confirmed that the drug is slowly released from the nanocomposite hydrogels. The results showed that starch-based nanocomposite hydrogels could provide appropriate repairing potential for defects exposed to changeable parameters. 相似文献
11.
A Dual‐Crosslinked Strategy to Construct Physical Hydrogels with High Strength,Toughness, Good Mechanical Recoverability,and Shape‐Memory Ability
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Zhihui Qin Rui Niu Chenjue Tang Jun Xia Feng Ji Dianyu Dong Haitao Zhang Shuo Zhang Junjie Li Fanglian Yao 《大分子材料与工程》2018,303(2)
A novel type of physical hydrogel based on dual‐crosslinked strategy is successfully synthesized by micellar copolymerization of stearyl methacrylate, acrylamide, and acrylic acid, and subsequent introduction of Fe3+. Strong hydrophobic associations among poly(stearyl methacrylate) blocks form the first crosslinking point and ionic coordination bonds between carboxyl groups and Fe3+ serve as the second crosslinking point. The mechanical properties of the hydrogel can be tuned in a wide range by controlling the densities of two crosslinks. The optimal hydrogel shows excellent mechanical properties (tensile strength of ≈6.8 MPa, elastic modulus of ≈8.0 MPa, elongation of ≈1000%, toughness of 53 MJ m?3) and good self‐recovery property. Furthermore, owing to stimuli responsiveness of physical interaction, this hydrogel also shows a triple shape memory effect. The combination of two different physical interactions in a single network provides a general strategy for designing of high‐strength hydrogels with functionalities. 相似文献
12.
Yizhe Liu Yang Wu Kai Feng Hui Liu Chenxi Qin Meirong Cai Xiaowei Pei Feng Zhou 《应用聚合物科学杂志》2024,141(16):e55264
In this work, a hydrophobic guest monomer containing adamant end-group was synthesized and introduced into the acrylamide hydrogel system to prepare macroscopic guest hydrogel. The swelling, transparency, and mechanical properties of the guest hydrogels can be significantly changed by soaking the guest hydrogel into hydrophilic cyclodextrin solution because the hydrophobic guest groups were recognized and covered by the hydrophilic host molecules. In addition, the surface lubrication property could be adjusted by changing the proportion of acrylamide and adamantane monomers in the hydrogel system. More importantly, cyclodextrin can bind with adamantane through host-guest interactions, enabling the adjustment of the hydrophilicity/hydrophobicity properties of the hydrogel system. By controlling the assembly time, the hydrogel with different lubrication behaviors can be obtained. The controllable surface friction that this specific binding of host-guest interaction has broad application prospects in intelligent device, bionic lubrication and other fields. 相似文献
13.
Raman spectroscopy was used to investigate molecular interactions and structure of water in PVME hydrogels of various crosslinking degrees. Analysis of polymer ν(CH3) and ν(CH2) stretching vibrations has allowed to monitor the changes of hydrophilic and hydrophobic polymer–water interactions in a course of water deswelling and volume phase transition. Formation of water–polymer hydrogen bonds has appeared to influence directly supramolecular structure of the absorbed water. It was found that the polymer network density determines an availability of the hydrophilic sites to water molecules and also influences the kinetics of volume phase transition of the hydrogels. Activation energy of the volume phase transition in the investigated systems was estimated to be ca.88 kJ/mol. 相似文献
14.
Prachishree Panda Agniva Dutta Debabrata Ganguly Santanu Chattopadhyay Rajat K. Das 《应用聚合物科学杂志》2020,137(48):49590
In this contribution, hydrophobic association and metal-ligand coordination have been employed in a dual physical crosslinking strategy to access hydrogels based on micellar copolymerization of acrylamide and a hydrophobic acrylic monomer (containing terpyridine (terpy) for metal-ligand interaction). The mechanical properties of these hydrogels are strongly influenced by the thermodynamic stability and kinetic lability of the metal-terpy crosslinks present in these materials. While the hydrogel tensile strength and stability on water exposure are enhanced by choosing stronger Fe2+-terpy crosslinks, the weaker and more kinetically labile Zn2+-terpy coordination bonds enable significantly higher energy dissipation under tensile loading and self-healing in the resultant hydrogels. 相似文献
15.
A classical ionic inorganic complex Na2[Cu(mnt)2] (mnt2− = maleonitriledithiolate = 1,2-dicyanoethylenedithiolate), that acts as a template in assembling neutral [Cu(salen)] (salen = bis(salicylidene)ethylenediamine) complexes forming a framework type arrangement, is accommodated in the channel formed in the crystal structure of a new type of host–guest compound [Cu(salen)]4 · Na2[Cu(mnt)2] (1). The non-covalent supramolecular interactions among [Cu(salen)] complexes and between [Cu(salen)] and [Cu(mnt)2]2− complexes in the crystal lattice of 1 result in weak antiferromagnetic coupling. 相似文献
16.
《Progress in Polymer Science》2014,39(12):1973-1986
Regenerative medicine involves interdisciplinary biomimetic approaches for cell therapy and tissue regeneration, employing the triad of cells, signals, and/or scaffolds. Remarkably, the field of therapeutic cells has evolved from the use of embryonic and adult stem cells to the use of induced pluripotent stem cells. For application of these cells in regenerative medicine, cell fate needs to be carefully controlled via external signals, such as the physical properties of an artificial extracellular matrix (ECM) and biologically active molecules in the form of small molecules, peptides, and proteins. It is therefore crucial to develop biomimetic scaffolds, reflecting the nanoenvironment of three-dimensional (3D) ECM in the body. Here, we describe in situ-forming injectable hydrogel systems, prepared using a variety of chemical crosslinkers and/or physical interactions, for application in regenerative medicine. Selective and fast chemical reactions under physiological conditions are prerequisites for in situ formation of injectable hydrogels. These hydrogels are attractive for regenerative medicine because of their ease of administration, facile encapsulation of cells and biomolecules without severe toxic effects, minimally invasive treatment, and possibly enhanced patient compliance. Recently, the Michael addition reaction between thiol and vinyl groups, the click reaction between bis(yne) molecules and multiarm azides, and the Schiff base reaction have been investigated for generation of injectable hydrogels, due to the high selectivity and biocompatibility of these reactions. Noncovalent physical interactions have also been proposed as crosslinking mechanisms for in situ forming injectable hydrogels. Hydrophobic interactions, ionic interactions, stereocomplex formation, complementary pair formation, and host–guest interactions drive the formation of 3D polymeric networks. In particular, supramolecular hydrogels have been developed using the host–guest chemistry of cyclodextrin (CD) and cucurbituril (CB), which allows highly selective, simple, and biocompatible crosslinking. Molecular recognition and complex formation of supramolecules, without the need for additional additives, have been successfully applied to the 3D network formation of polymer chains. Finally, we review the current state of the art of injectable hydrogel systems for application in regenerative medicine, including cell therapy and tissue regeneration. 相似文献
17.
Hans Wolfgang Spiess 《Israel journal of chemistry》2014,54(1-2):16-24
Sideband patterns in single quantum and double quantum magic angle spinning NMR spectra are reviewed. Their use in elucidating non-covalent interactions, such as hydrogen bonds or pi-pi stacking, is demonstrated by studies of supramolecular systems of current interest. Moreover, the effects of local and collective motions are illustrated by examples from supramolecular and macromolecular science. 相似文献
18.
Enzymatic hydrogelation of small molecules 总被引:1,自引:0,他引:1
Enzymes, a class of highly efficient and specific catalysts in Nature, dictate a myriad of reactions that constitute various cascades in biological systems. Self-assembly, a process prevalent in Nature, also plays important roles in biology, from maintaining the integrity of cells to performing cellular functions and inducing abnormalities that cause disease. To explore enzyme-regulated molecular self-assembly in an aqueous medium will help to understand and control those important biological processes. On the other hand, certain small organic molecules self-assemble in water to form molecular nanofibers and result in a hydrogel, which is referred to as a "supramolecular hydrogel" (and the small molecules are referred to as "supramolecular hydrogelators"). Supramolecular hydrogelators share common features, such as amphiphilicity and supramolecular interactions (pi-pi interactions, hydrogen bonding, and charge interactions among the molecules, among others) that result in nanostructures and form the three-dimensional networks as the matrices of hydrogels. In this Account, we discuss the use of enzymes to trigger and control the self-assembly of small molecules for hydrogelation, which takes place in vitro or in vivo, extra- or intracellularly. Using phosphatase, thermolysin, beta-lactamase, and phosphatase/kinase as examples, we illustrate the design and application of enzyme-catalyzed or -regulated formation of supramolecular hydrogels that offer a new strategy for detecting the activity of enzymes, screening for enzyme inhibitors, typing bacteria, drug delivery systems, and controlling the fate of cells. Since the expression and distribution of enzymes differ by the types and states of cells, tissues, and organs, using an enzymatic reaction to convert precursors into hydrogelators that self-assemble into nanofibers as the matrices of the hydrogel, one can control the delivery, function, and response of a hydrogel according to a specific biological condition or environment, thus providing an accessible route to create sophisticated materials for biomedicine. Particularly, intracellular enzymatic hydrogelation of small molecules offers a unique means for scientists to integrate molecular self-assembly with inherent enzymatic reactions inside cells for developing new biomaterials and therapeutics at the supramolecular level and improving the basic understanding of dynamic molecular self-assembly in water. 相似文献
19.
稳定的活性物载体--葡糖微球 总被引:1,自引:0,他引:1
系统介绍了法国蔻波公司研制开发的一种新型释放体系-葡糖微球。葡糖微球具有独物的仿生结构-围绕一个固态内核排列的超分子,分别通过离子链和疏水作用来包裹和保护亲油性和亲水性的化妆品洗性成分。经测试具有优异的防止如维生素或酶等易变分子的降解,保持被包裹物活性的功效。因其独特的释放体系,很小的粒径被成功地应用于表皮上层活性成分的保持和传输。 相似文献
20.
Hyeon Jeong Kang Nare Ko Seung Jun Oh Seong Yeong An Yu-Shik Hwang So Yeon Kim 《International journal of molecular sciences》2021,22(24)
Traumatic injury of the oral cavity is atypical and often accompanied by uncontrolled bleeding and inflammation. Injectable hydrogels have been considered to be promising candidates for the treatment of oral injuries because of their simple formulation, minimally invasive application technique, and site-specific delivery. Fibrinogen-based hydrogels have been widely explored as effective materials for wound healing in tissue engineering due to their uniqueness. Recently, an injectable foam has taken the spotlight. However, the fibrin component of this biomaterial is relatively stiff. To address these challenges, we created keratin-conjugated fibrinogen (KRT-FIB). This study aimed to develop a novel keratin biomaterial and assess cell–biomaterial interactions. Consequently, a novel injectable KRT-FIB hydrogel was optimized through rheological measurements, and its injection performance, swelling behavior, and surface morphology were investigated. We observed an excellent cell viability, proliferation, and migration/cell–cell interaction, indicating that the novel KRT-FIB-injectable hydrogel is a promising platform for oral tissue regeneration with a high clinical applicability. 相似文献