Structure and gelation properties of thermoresponsive bottlebrush hydrogels

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Structure and gelation properties of thermoresponsive bottlebrush hydrogels

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In this study, polyurethane (PU) hydrogels were synthesized via mercapto curing reaction to elucidate the effect of molecular interactions between isocyanate and soft segments on the properties of hydrogels. Further, the mesh size, mechanical properties, hydrophilicity, and biological properties of the PU hydrogels were determined. In the isocyanate series, the structural regularity and rigidity of 4,4′‐dicyclohexylmethane diisocyanate (HMDI) favored the formation of hydrogel materials with small mesh size, high modulus, and low water absorption. In contrast, l‐lysine diisocyanate (LDI) favored the materials with large mesh size, low modulus, and good hydrophilicity. In the soft‐segment series, the strong hydrogen bonds of polycarbonate diol (PCDL) favored the formation of materials with small mesh size, dense cross‐link points, and high modulus, whereas weak hydrogen bonds of polytetrahydrofuran ether glycol (PTMG) favored the hydrogel materials with small mesh size, few crosslink points, and low modulus. PU hydrogels exhibit excellent cytocompatibility, anti‐cell adhesion, and anti‐inflammatory properties. Therefore, this study offers valuable insights into understanding the chain structure and macroscopic properties, thus contributing to preparing PU hydrogels with varying performances, as desired.

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Fabrication of composite hydrogels by assembly of okara cellulose nanofibers and gum Arabic in ionic liquids: Structure and properties
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Thermo-Responsive Poly(N-Isopropylacrylamide)-Cellulose Nanocrystals Hybrid Hydrogels for Wound Dressing
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Thermo-responsive hydrogels containing poly(N-isopropylacrylamide) (PNIPAAm), reinforced both with covalent and non-covalent interactions with cellulose nanocrystals (CNC), were synthesized via free-radical polymerization in the absence of any additional cross-linkers. The properties of PNIPAAm-CNC hybrid hydrogels were dependent on the amounts of incorporated CNC. The thermal stability of the hydrogels decreased with increasing CNC content. The rheological measurement indicated that the elastic and viscous moduli of hydrogels increased with the higher amounts of CNC addition, representing stronger mechanical properties of the hydrogels. Moreover, the hydrogel injection also supported the hypothesis that CNC reinforced the hydrogels; the increased CNC content exhibited higher structural integrity upon injection. The PNIPAAm-CNC hybrid hydrogels exhibited clear thermo-responsive behavior; the volume phase transition temperature (VPTT) was in the range of 36 to 39 °C, which is close to normal human body temperature. For wound dressing purposes, metronidazole, an antibiotic and antiprotozoal often used for skin infections, was used as a target drug to study drug-loading and the release properties of the hydrogels. The hydrogels showed a good drug-loading capacity at room temperature and a burst drug release, which was followed by slow and sustained release at 37 °C. These results suggested that newly developed drugs containing injectable hydrogels are promising materials for wound dressing.

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Highly absorbent hydrogels comprised from interpenetrated networks of alginate\u2013polyurethane for biomedical applications
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Developing new approaches to improve the swelling, degradation rate, and mechanical properties of alginate hydrogels without compromising their biocompatibility for biomedical applications represents a potential area of research. In this work, the generation of interpenetrated networks (IPN) comprised from alginate–polyurethane in an aqueous medium is proposed to design hydrogels with tailored properties for biomedical applications. Aqueous polyurethane (PU) dispersions can crosslink and interpenetrate alginate chains, forming amide bonds that allow the structure and water absorption capacity of these novel hydrogels to be regulated. In this sense, this work focuses on studying the relation of the PU concentration on the properties of these hydrogels. The results indicate that the crosslinking of the alginate with PU generates IPN hydrogels with a crystalline structure characterized by a homogeneous smooth surface with high capacity to absorb water, tailoring the degradation rate, thermal decomposition, and storage module, not altering the native biocompatibility of alginate, providing character to inhibit the growth of E. coli and increasing also its hemocompatibility. The IPN hydrogels that include 20 wt.% of PU exhibit a reticulation index of 46 ± 4%, swelling capacity of 545 ± 13% at 7 days of incubation at physiological pH, resistance to both acidic and neutral hydrolytic degradation, mechanical improvement of 91 ± 1%, and no cytotoxicity for monocytes and fibroblasts growing for up to 72 h of incubation. These results indicate that these novel hydrogels can be used for successful biomedical applications in the design of wound healing dressings.

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Structure and Properties of Hydrophobic Aggregation Hydrogel with Chemical Sensitive Switch
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  • International Journal of Polymer Science
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Hydrogels with chemical sensitive switch have control release properties in special environments. A series of polyacrylamide-octadecyl methacrylate hydrogels crosslinked by N,N′-bis (acryloyl) cystamine were synthesized as potential chemical sensitive system. When this hydrogel encounters dithiothreitol it can change its quality. The properties of the hydrogels were characterized by infrared spectroscopy, contact angle, and scanning electron microscopy. The water absorption of the hydrogel has the maximum value of 475%, when the content of octadecyl methacrylate is 5 wt%. The amount of weight loss was changed from 34.6% to 17.2%, as the content of octadecyl methacrylate increased from 3 wt% to 9.4 wt%. At the same time, the stress of the hydrogel decreased from 67.01% to 47.61%; the strength of the hydrogel reaches to the maximum 0.367 Mpa at 7 wt% octadecyl methacrylate. The increasing content of octadecyl methacrylate from 3 wt% to 9.4 wt% can enhance the hydrophobicity of the hydrogel; the contact angle of water to hydrogel changed from 14.10° to 19.62°. This hydrogel has the porous structure which permits loading of oils into the gel matrix. The functionalities of the hydrogel make it have more widely potential applications in chemical sensitive response materials.

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The tunable properties of thermoresponsive physical hydrogels recently found application in catalysis. The most relevant examples are described in this perspective article. Novel concepts are especially highlighted through the beneficial effects of thermoresponsive hydrogels on the catalytic performance. Their scope and future developments are also addressed.

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Mechanical properties, structure, bioadhesion, and biocompatibility of pectin hydrogels.
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The surface structure, biocompatibility, textural, and adhesive properties of calcium hydrogels derived from 1, 2, and 4% solutions of apple pectin were examined in this study. An increase in the pectin concentration in hydrogels was shown to improve their stability toward elastic and plastic deformation. The elasticity of pectin hydrogels, measured as Young's modulus, ranged from 6 to 100 kPa. The mechanical properties of the pectin hydrogels were shown to correspond to those of soft tissues. The characterization of surface roughness in terms of the roughness profile (Ra) and the root-mean-square deviation of the roughness profile (Rq) indicated an increased roughness profile for hydrogels depending on their pectin concentration. The adhesion of AU2% and AU4% hydrogels to the serosa abdominal wall, liver, and colon was higher than that of the AU1% hydrogel. The adhesion of macrophages and the non-specific adsorption of blood plasma proteins were found to increase as the pectin concentration in the hydrogels increased. The rate of degradation of all hydrogels was higher in phosphate buffered saline (PBS) than that in DMEM and a fibroblast cell monolayer. The pectin hydrogel was also found to have a low cytotoxicity. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 105A: 2572-2581, 2017.

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Properties of Thermoresponsive N-maleyl gelatin-co-P(N-isopropylacrylamide) hydrogel with ultrahigh mechanical strength and self-recovery
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Thermo-responsive polymer hydrogels with superior strength and toughness are potential candidate materials in biomedical field, such as drug delivery system and tissue engineering. By introducing maleylgelatin (MAGEL) into the conventional PNIPAAm hydrogel, a series of composite P(NIPAAm-co-MAGEL) hydrogels with combined features were fabricated. Thermo-responsive behaviors, equilibrium swelling ratio (ESR), compression strength, tensile strength (TS) and elongation at-break (E), cyclic compression tests, and thermal stability properties of hydrogels with different amount of MAGEL were investigated. Experimental data indicated that the amount of MAGEL could modulate the mechanical property of the composite hydrogel. With the increase of the MAGEL contents from 0 to 50%, the composite hydrogel with relatively high water content possessed good compressive strength, tensile strength and stretrability. Only when the weight ratio of MAGEL/NIPAAm was 30:70, did the P(NIPAAm-co-MAGEL) have a homogeneous distribution and stable 3D networks which played a significant role in the properties of the hydrogels. Cyclic compression tests results indicated that P(NIPAAm-co-MAGEL) hydrogel had an excellent thermo-reversible ability. This research would expand the scope of the PNIPAAm hydrogel applications.

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Smart hydrogel-functionalized textile system with moisture management property for skin application
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In this study, a functional textile-based material for topical skin application was fabricated by coating a thermoresponsive hydrogel onto one side of absorbent nonwoven fabric. The thermoresponsive hydrogel was synthesized easily through coupling of poly (ethylene glycol) (PEG) and poly (ϵ-caprolactone) (PCL) with hexamethylene diisocyanate (HMDI) as a chemical linker. The chemical structure of the as-prepared triblock copolymer hydrogel was unraveled by FTIR and 1H NMR analysis. The hydrogel showed a temperature-triggered sol-gel transition behavior and high potential for use as drug controlled release. When the surrounding temperature was close to the skin temperature of around 34 °C, it became a moisture management system where the liquids including sweat, blood, and other body fluids can be transported unidirectionally from one fabric side with the hydrophobic hydrogel coating to the untreated opposite side. This thereby showed that the thermoresponsive hydrogel-coated textile materials had a function to keep topical skin area clean, breathable, and comfortable, thus suggesting a great potential and significance for long-term skin treatment application. The structure and surface morphology of the thermoresponsive hydrogel, in vitro drug release behavior, and the mechanism of unidirectional water transport were investigated in detail. Our success in preparation of the functional textile composites will pave the way for development of various polymer- or textile-based functional materials that are applicable in the real world.

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Impact of Hofmeister anion type on the structural and mechanical properties of composite whey protein hydrogels

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