Pullulan-based composite scaffolds for bone tissue engineering: Improved osteoconductivity by pore wall mineralization.

PubMed

Amrita; Arora, Aditya; Sharma, Poonam; Katti, Dhirendra S

2015-06-05

Porous hydrogels have been explored for bone tissue engineering; however their poor mechanical properties make them less suitable as bone graft substitutes. Since incorporation of fillers is a well-accepted method for improving mechanical properties of hydrogels, in this work pullulan hydrogels were reinforced with nano-crystalline hydroxyapatite (nHAp) (5 wt% nHAp in hydrogel) and poly(3-hydroxybutyrate) (PHB) fibers (3 wt% fibers in hydrogel) containing nHAp (3 wt% nHAp in fibers). Addition of these fillers to pullulan hydrogel improved compressive modulus of the scaffold by 10 fold. However, the hydrophilicity of pullulan did not support adhesion and spreading of cells. To overcome this limitation, porous composite scaffolds were modified using a double diffusion method that enabled deposition of hydroxyapatite on pore walls. This method resulted in rapid and uniform coating of HAp throughout the three-dimensional scaffolds which not only rendered them osteoconductive in vitro but also led to an improvement in their compressive modulus. These results demonstrate the potential of mineralized pullulan-based composite scaffolds in non-load bearing bone tissue engineering. Copyright © 2015 Elsevier Ltd. All rights reserved.

Spatiotemporal Programing for the On-Demand Release of Bupivacaine Based on an Injectable Composite Hydrogel.

PubMed

Dinh, Van Vuong; Suh, Yun-Suhk; Yang, Han-Kwang; Lim, Yong Taik

2016-12-01

We report a programed drug delivery system that can tailor the release of anesthetic bupivacaine in a spatiotemporally controlled manner. The drug delivery system was developed through the combination of a collagen-based injectable hydrogel and 2 types of poly(lactic-co-glycolic acid) (PLGA) particles. As a rapid-release platform (90% release after 24 h), bupivacaine hydrochloride was incorporated into collagen/poly(γ-glutamic acid) hydrogel, which exhibited gel formation at body temperature. PLGA microparticles (diameter 1-3 μm) containing bupivacaine base showed a very slow release of bupivacaine (95% after 240 h), whereas PLGA nanoparticles (124 ± 30 nm) containing bupivacaine base demonstrated an intermediate release rate (95% after 160 h). By changing the relative composition ratio between the 3 components in these injectable composite hydrogels, the release of bupivacaine could be easily controlled from very rapid (within 1 day) to very delayed (up to 9 days). The experimental results on the release data (cumulative release, time point release, average release rate) were coincident with the release profile generated by computer simulation. These injectable composite hydrogels with systematically tunable mixing ratios are expected to serve as a promising technology for the on-demand release of bupivacaine in pain management. Copyright © 2016 American Pharmacists Association®. Published by Elsevier Inc. All rights reserved.

Polyluminol/hydrogel composites as new electrochemiluminescent-active sensing layers.

PubMed

Leca-Bouvier, Béatrice D; Sassolas, Audrey; Blum, Loïc J

2014-09-01

This paper reports on electrochemiluminescent sensors and biosensors based on polyluminol/hydrogel composite sensing layers using chemical or biological membranes as hydrogel matrices. In this work, luminol is electropolymerized under near-neutral conditions onto screen-printed electrode (SPE)-supported hydrogel films. The working electrode coated with a hydrogel film is soaked in a solution containing monomeric luminol units, allowing the monomeric luminol units to diffuse inside the porous matrix to the electrode surface where they are electropolymerized by cyclic voltammetry (CV). Sensors and enzymatic biosensors for H2O2 and choline detection, respectively, have been developed, using choline oxidase (ChOD) as a model enzyme. In this case, hydrogel is used both as the enzymatic immobilization matrix and as a template for the electrosynthesis of polyluminol. The enzyme was immobilized by entrapment in the gel matrix during its formation before electropolymerization of the monomer. Several parameters have been optimized in terms of polymerization conditions, enzyme loading, and average pore size. Using calcium alginate or tetramethoxysilane (TMOS)-based silica as porous matrix, H2O2 and choline detection are reported down to micromolar concentrations with three orders of magnitude wide dynamic ranges starting from 4 × 10(-7) M. Polyluminol/hydrogel composites appear as suitable electrochemiluminescence (ECL)-active sensing layers for the design of new reagentless and disposable easy-to-use optical sensors and biosensors, using conventional TMOS-based silica gel or the more original and easier to handle calcium alginate, reported here for the first time in such a configuration, as the biocompatible hydrogel matrix.

Radiation synthesis of superabsorbent CMC based hydrogels for agriculture applications

NASA Astrophysics Data System (ADS)

Raafat, Amany I.; Eid, Mona; El-Arnaouty, Magda B.

2012-07-01

A series of superabsorbent hydrogel based on carboxymethylcellulose (CMC) and polyvinylpyrrolidone (PVP) crosslinked with gamma irradiation have been proposed for agriculture application. The effect of preparation conditions such as feed solution composition and absorbed irradiation dose on the gelation and swelling degree was evaluated. The structure and the morphology of the superabsorbent CMC/PVP hydrogel were characterized using Fourier transform infrared spectroscopy technique (FTIR), and scanning electron microscope (SEM). Effect of ionic strength and cationic and anionic kinds on the swelling behavior of the obtained hydrogel was investigated. Urea as an agrochemical model was loaded onto the obtained hydrogel to provide nitrogen (N) nutrients. The water retention capability and the urea release behavior of the CMC/PVP hydrogels were investigated. It was found that, the obtained CMC/PVP hydrogels have good swelling degree that greatly affected by its composition and absorbed dose. The swelling was also extremely sensitive to the ionic strength and cationic kind. Owing to its considerable slow urea release, good water retention capacity, being economical, and environment-friendly, it might be useful for its application in agriculture field.

Surface wettability enhancement of silicone hydrogel lenses by processing with polar plastic molds.

PubMed

Lai, Y C; Friends, G D

1997-06-05

In the quest for hydrogel contact lenses with improved extended wear capability, the use of siloxane moieties in the lens materials was investigated. However, the introduction of hydrophobic siloxane groups gave rise to wettability and lipidlike deposit problems. It was found that when polysiloxane-based compositions for hydrogels were processed with polar plastic molds, such as those fabricated from an acrylonitrile-based polymer, the hydrogel lenses fabricated were wettable, with minimized lipidlike deposits. These findings were supported by the wettability of silicone hydrogel films, silicon, and nitrogen element contents near lens surfaces, as well as the results from clinical assessment of silicone hydrogel lenses.

Effects of halloysite nanotubes on physical properties and cytocompatibility of alginate composite hydrogels.

PubMed

Huang, Biao; Liu, Mingxian; Long, Zheru; Shen, Yan; Zhou, Changren

2017-01-01

Sodium alginate (SA)/halloysite nanotubes (HNTs) composite hydrogels were successfully prepared by solution blending and cross-linking with calcium ions. HNTs can improve the physical properties and cytocompatibility of composite hydrogels. The static and shear viscosity of SA/HNTs solution increase by the addition of HNTs. FTIR suggests the presence of hydrogen bond interactions between HNTs and SA. The crystal structure of HNTs is retained in the composites as showed by the X-ray diffraction result. A porous structure with pore size of 100-250μm is found in the hydrogels, which can provide a space for cell growth and migration. The compressive mechanical properties of composite hydrogels significantly increase compared to the pure SA hydrogel. The SA/HNTs composite hydrogels with 80% HNTs loading exhibit the compressive stress at 80% strain of 2.99MPa, while the stress at 80% strain of pure SA hydrogel is only 0.8MPa. The dynamic storage modulus of composite hydrogels also markedly increases with HNTs concentration. The differential scanning calorimetry endothermic peak area and swelling ratios in NaCl solution of the composite hydrogels decrease by the addition of HNTs. Preosteoblast (MC3T3-E1) culture results reveal that the SA/HNTs composites especially at relatively low HNTs loading show a significant increase in cells adhesion and proliferation compared to the pure SA hydrogel. All the results demonstrate that the SA/HNTs composite hydrogels show a promising application in bone tissue engineering. Copyright © 2016 Elsevier B.V. All rights reserved.

Chitosan composite hydrogels reinforced with natural clay nanotubes.

PubMed

Huang, Biao; Liu, Mingxian; Zhou, Changren

2017-11-01

Here, chitosan composites hydrogels were prepared by addition of halloysite nanotubes (HNTs) in the chitosan KOH/LiOH/urea solution. The raw chitosan and chitosan/HNTs composite hydrogels were obtained by heat treatment at 60°C for 8h and then regeneration in ethanol solution. The viscosity of the composite solution is increased with HNTs content. The Fourier transform infrared spectroscopy (FT-IR) shows that the hydrogen bonds interactions exist between the HNTs and the chitosan. X-ray diffraction (XRD) results show that the crystal structure of HNT is not changed in the composite hydrogels. The compressive property test and storage modulus determination show that the mechanical properties and anti-deformation ability of the composite hydrogel significantly increase owing to the reinforcing effect of HNTs. The composites hydrogel with 66.7% HNTs can undergo 7 times compression cycles without breaking with compressive strength of 0.71MPa at 70% deformation, while pure chitosan hydrogel is broken after bearing 5 compression cycles with compressive strength of 0.14MPa and a maximum deformation of 59%. A porous structure with pore size of 100-500μm is found in the composite hydrogels by scanning electron microscopy (SEM), and the pore size and the swelling ratio in NaCl solution decrease by the addition of HNTs and the immersing of ethanol. Chitosan/HNTs composite hydrogels show low cytotoxicity towards MC3T3-E1 cells. Also, the composite hydrogels show a maximum drug entrapment efficiency of 45.7% for doxorubicin (DOX) which is much higher than that of pure chitosan hydrogel (27.5%). All the results illustrate that the chitosan/HNTs composite hydrogels show promising applications as biomaterials. Copyright © 2017 Elsevier Ltd. All rights reserved.

Self-assembled high-strength hydroxyapatite/graphene oxide/chitosan composite hydrogel for bone tissue engineering.

PubMed

Yu, Peng; Bao, Rui-Ying; Shi, Xiao-Jun; Yang, Wei; Yang, Ming-Bo

2017-01-02

Graphene hydrogel has shown greatly potentials in bone tissue engineering recently, but it is relatively weak in the practical use. Here we report a facile method to synthesize high strength composite graphene hydrogel. Graphene oxide (GO), hydroxyapatite (HA) nanoparticles (NPs) and chitosan (CS) self-assemble into a 3-dimensional hydrogel with the assistance of crosslinking agent genipin (GNP) for CS and reducing agent sodium ascorbate (NaVC) for GO simultaneously. The dense and oriented microstructure of the resulted composite gel endows it with high mechanical strength, high fixing capacity of HA and high porosity. These properties together with the good biocompatibility make the ternary composite gel a promising material for bone tissue engineering. Such a simultaneous crosslinking and reduction strategy can also be applied to produce a variety of 3D graphene-polymer based nanocomposites for biomaterials, energy storage materials and adsorbent materials. Copyright © 2016 Elsevier Ltd. All rights reserved.

Smart nanocomposite hydrogels based on azo crosslinked graphene oxide for oral colon-specific drug delivery

NASA Astrophysics Data System (ADS)

Hou, Lin; Shi, Yuyang; Jiang, Guixiang; Liu, Wei; Han, Huili; Feng, Qianhua; Ren, Junxiao; Yuan, Yujie; Wang, Yongchao; Shi, Jinjin; Zhang, Zhenzhong

2016-08-01

A safe and efficient nanocomposite hydrogel for colon cancer drug delivery was synthesized using pH-sensitive and biocompatible graphene oxide (GO) containing azoaromatic crosslinks as well as poly (vinyl alcohol) (PVA) (GO-N=N-GO/PVA composite hydrogels). Curcumin (CUR), an anti-cancer drug, was encapsulated successfully into the hydrogel through a freezing and thawing process. Fourier transform infrared spectroscopy, scanning electron microscopy and Raman spectroscopy were performed to confirm the formation and morphological properties of the nanocomposite hydrogel. The hydrogels exhibited good swelling properties in a pH-sensitive manner. Drug release studies under conditions mimicking stomach to colon transit have shown that the drug was protected from being released completely into the physiological environment of the stomach and small intestine. In vivo imaging analysis, pharmacokinetics and a distribution of the gastrointestinal tract experiment were systematically studied and evaluated as colon-specific drug delivery systems. All the results demonstrated that GO-N=N-GO/PVA composite hydrogels could protect CUR well while passing through the stomach and small intestine to the proximal colon, and enhance the colon-targeting ability and residence time in the colon site. Therefore, CUR loaded GO-N=N-GO/PVA composite hydrogels might potentially provide a theoretical basis for the treatment of colon cancer with high efficiency and low toxicity.

Development of a P((MAA-co-NVP)-g-EG) Hydrogel Platform for Oral Protein Delivery: Effects of Hydrogel Composition on Environmental Response and Protein Partitioning.

PubMed

Steichen, Stephanie; O'Connor, Colleen; Peppas, Nicholas A

2017-01-01

Hydrogels based upon terpolymers of methacrylic acid, N-vinyl pyrrolidone, and poly(ethylene glycol) are developed and characterized for their ability to respond to changes in environmental pH and to partition protein therapeutics of varying molecular weights and isoelectric points. P((MAA-co-NVP)-g-EG) hydrogels are synthesized with PEG-based cross-linking agents of varying length and incorporation densities. The composition is confirmed using FT-IR spectroscopy and shows peak shifts indicating hydrogen bonding. Scanning electron microscopy reveals microparticles with an irregular, planar morphology. The pH-responsive behavior of the hydrogels is confirmed under equilibrium and dynamic conditions, with the hydrogel collapsed at acidic pH and swollen at neutral pH. The ability of the hydrogels to partition model protein therapeutics at varying pH and ionic strength is evaluated using three model proteins: insulin, porcine growth hormone, and ovalbumin. Finally, the microparticles are evaluated for adverse interactions with two model intestinal cell lines and show minimal cytotoxicity at concentrations below 5 mg mL -1 . © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Thermo-responsive methylcellulose hydrogels as temporary substrate for cell sheet biofabrication.

PubMed

Altomare, Lina; Cochis, Andrea; Carletta, Andrea; Rimondini, Lia; Farè, Silvia

2016-05-01

Methylcellulose (MC), a water-soluble polymer derived from cellulose, was investigated as a possible temporary substrate having thermo-responsive properties favorable for cell culturing. MC-based hydrogels were prepared by a dispersion technique, mixing MC powder (2, 4, 6, 8, 10, 12 % w/v) with selected salts (sodium sulphate, Na2SO4), sodium phosphate, calcium chloride, or phosphate buffered saline, to evaluate the influence of different compositions on the thermo-responsive behavior. The inversion test was used to determine the gelation temperatures of the different hydrogel compositions; thermo-mechanical properties and thermo-reversibility of the MC hydrogels were investigated by rheological analysis. Gelation temperatures and rheological behavior depended on the MC concentration and type and concentration of salt used in hydrogel preparation. In vitro cytotoxicity tests, performed using L929 mouse fibroblasts, showed no toxic release from all the tested hydrogels. Among the investigated compositions, the hydrogel composed of 8 % w/v MC with 0.05 M Na2SO4 had a thermo-reversibility temperature at 37 °C. For that reason, this formulation was thus considered to verify the possibility of inducing in vitro spontaneous detachment of cells previously seeded on the hydrogel surface. A continuous cell layer (cell sheet) was allowed to grow and then detached from the hydrogel surface without the use of enzymes, thanks to the thermo-responsive behavior of the MC hydrogel. Immunofluorescence observation confirmed that the detached cell sheet was composed of closely interacting cells.

Photo-cross-linkable methacrylated gelatin and hydroxyapatite hybrid hydrogel for modularly engineering biomimetic osteon.

PubMed

Zuo, Yicong; Liu, Xiaolu; Wei, Dan; Sun, Jing; Xiao, Wenqian; Zhao, Huan; Guo, Likun; Wei, Qingrong; Fan, Hongsong; Zhang, Xingdong

2015-05-20

Modular tissue engineering holds great potential in regenerating natural complex tissues by engineering three-dimensional modular scaffolds with predefined geometry and biological characters. In modular tissue-like construction, a scaffold with an appropriate mechanical rigidity for assembling fabrication and high biocompatibility for cell survival is the key to the successful bioconstruction. In this work, a series of composite hydrogels (GH0, GH1, GH2, and GH3) based on a combination of methacrylated gelatin (GelMA) and hydroxyapatite (HA) was exploited to enhance hydrogel mechanical rigidity and promote cell functional expression for osteon biofabrication. These composite hydrogels presented a lower swelling ratio, higher mechanical moduli, and better biocompatibility when compared to the pure GelMA hydrogel. Furthermore, on the basis of the composite hydrogel and photolithograph technology, we successfully constructed an osteon-like concentric double-ring structure in which the inner ring encapsulating human umbilical vascular endothelial cells (HUVECs) was designed to imitate blood vessel tubule while the outer ring encapsulating human osteoblast-like cells (MG63s) acts as part of bone. During the coculture period, MG63s and HUVECs exhibited not only satisfying growth status but also the enhanced genic expression of osteogenesis-related and angiogenesis-related differentiations. These results demonstrate this GelMA-HA composite hydrogel system is promising for modular tissue engineering.

Viscoelastic behaviour of hydrogel-based composites for tissue engineering under mechanical load.

PubMed

Kocen, Rok; Gasik, Michael; Gantar, Ana; Novak, Saša

2017-03-06

Along with biocompatibility, bioinductivity and appropriate biodegradation, mechanical properties are also of crucial importance for tissue engineering scaffolds. Hydrogels, such as gellan gum (GG), are usually soft materials, which may benefit from the incorporation of inorganic particles, e.g. bioactive glass, not only due to the acquired bioactivity, but also due to improved mechanical properties. They exhibit complex viscoelastic properties, which can be evaluated in various ways. In this work, to reliably evaluate the effect of the bioactive glass (BAG) addition on viscoelastic properties of the composite hydrogel, we employed and compared the three most commonly used techniques, analyzing their advantages and limitations: monotonic uniaxial unconfined compression, small amplitude oscillatory shear (SAOS) rheology and dynamic mechanical analysis (DMA). Creep and small amplitude dynamic strain-controlled tests in DMA are suggested as the best ways for the characterization of mechanical properties of hydrogel composites, whereas the SAOS rheology is more useful for studying the hydrogel's processing kinetics, as it does not induce volumetric changes even at very high strains. Overall, the results confirmed a beneficial effect of BAG (nano)particles on the elastic modulus of the GG-BAG composite hydrogel. The Young's modulus of 6.6 ± 0.8 kPa for the GG hydrogel increased by two orders of magnitude after the addition of 2 wt.% BAG particles (500-800 kPa).

A composite hydrogels-based photonic crystal multi-sensor

NASA Astrophysics Data System (ADS)

Chen, Cheng; Zhu, Zhigang; Zhu, Xiangrong; Yu, Wei; Liu, Mingju; Ge, Qiaoqiao; Shih, Wei-Heng

2015-04-01

A facile route to prepare stimuli-sensitive poly(vinyl alcohol)/poly(acrylic acid) (PVA/PAA) gelated crystalline colloidal array photonic crystal material was developed. PVA was physically gelated by utilizing an ethanol-assisted method, the resulting hydrogel/crystal composite film was then functionalized with PAA to form an interpenetrating hydrogel film. This sensor film is able to efficiently diffract the visible light and rapidly respond to various environmental stimuli such as solvent, pH and strain, and the accompanying structural color shift can be repeatedly changed and easily distinguished by naked eye.

Design and characterization of a biodegradable composite scaffold for ligament tissue engineering.

PubMed

Hayami, James W S; Surrao, Denver C; Waldman, Stephen D; Amsden, Brian G

2010-03-15

Herein we report on the development and characterization of a biodegradable composite scaffold for ligament tissue engineering based on the fundamental morphological features of the native ligament. An aligned fibrous component was used to mimic the fibrous collagen network and a hydrogel component to mimic the proteoglycan-water matrix of the ligament. The composite scaffold was constructed from cell-adherent, base-etched, electrospun poly(epsilon-caprolactone-co-D,L-lactide) (PCLDLLA) fibers embedded in a noncell-adherent photocrosslinked N-methacrylated glycol chitosan (MGC) hydrogel seeded with primary ligament fibroblasts. Base etching improved cellular adhesion to the PCLDLLA material. Cells within the MGC hydrogel remained viable (72 +/- 4%) during the 4-week culture period. Immunohistochemistry staining revealed ligament ECM markers collagen type I, collagen type III, and decorin organizing and accumulating along the PCLDLLA fibers within the composite scaffolds. On the basis of these results, it was determined that the composite scaffold design was a viable alternative to the current approaches used for ligament tissue engineering and merits further study. (c) 2009 Wiley Periodicals, Inc.

Self-Supporting Nanoclay as Internal Scaffold Material for Direct Printing of Soft Hydrogel Composite Structures in Air.

PubMed

Jin, Yifei; Liu, Chengcheng; Chai, Wenxuan; Compaan, Ashley; Huang, Yong

2017-05-24

Three dimensional (3D) bioprinting technology enables the freeform fabrication of complex constructs from various hydrogels and is receiving increasing attention in tissue engineering. The objective of this study is to develop a novel self-supporting direct hydrogel printing approach to extrude complex 3D hydrogel composite structures in air without the help of a support bath. Laponite, a member of the smectite mineral family, is investigated to serve as an internal scaffold material for the direct printing of hydrogel composite structures in air. In the proposed printing approach, due to its yield-stress property, Laponite nanoclay can be easily extruded through a nozzle as a liquid and self-supported after extrusion as a solid. Its unique crystal structure with positive and negative charges enables it to be mixed with many chemically and physically cross-linked hydrogels, which makes it an ideal internal scaffold material for the fabrication of various hydrogel structures. By mixing Laponite nanoclay with various hydrogel precursors, the hydrogel composites retain their self-supporting capacity and can be printed into 3D structures directly in air and retain their shapes before cross-linking. Then, the whole structures are solidified in situ by applying suitable cross-linking stimuli. The addition of Laponite nanoclay can effectively improve the mechanical and biological properties of hydrogel composites. Specifically, the addition of Laponite nanoclay results in a significant increase in the Young's modulus of each hydrogel-Laponite composite: 1.9-fold increase for the poly(ethylene glycol) diacrylate (PEGDA)-Laponite composite, 7.4-fold increase for the alginate-Laponite composite, and 3.3-fold increase for the gelatin-Laponite composite.

Degradation prediction model and stem cell growth of gelatin-PEG composite hydrogel.

PubMed

Zhou, Nan; Liu, Chang; Lv, Shijie; Sun, Dongsheng; Qiao, Qinglong; Zhang, Rui; Liu, Yang; Xiao, Jing; Sun, Guangwei

2016-12-01

Gelatin hydrogel has great potential in regenerative medicine. The degradation of gelatin hydrogel is important to control the release profile of encapsulated biomolecules and regulate in vivo tissue repair process. As a plasticizer, PEG can significantly improve the mechanical property of gelatin hydrogel. However, how preparation parameters affect the degradation rate of gelatin-PEG composite hydrogel is still not clear. In this study, the significant effect factor, glutaraldehyde (GA) concentration, was confirmed by means of Plackett-Burman method. Then a mathematical model was built to predict the degradation rate of composite hydrogels under different preparation conditions using the response surface method (RSM), which was helpful to prepare the certain composite hydrogel with desired degradation rate. In addition, it was found that gelatin-PEG composite hydrogel surface well supported the adhesion and growth of human mesenchymal stem cells (MSCs). Moreover, PEG concentration not only could adjust hydrogel degradation more subtly, but also might increase the cross-linking degree and affect the cell migration. Therefore, these results would be useful to optimize the preparation of gelatin-PEG composite hydrogel for drug delivery or tissue engineering. © 2016 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 104A: 3149-3156, 2016. © 2016 Wiley Periodicals, Inc.

A comparative study on collagen type I and hyaluronic acid dependent cell behavior for osteochondral tissue bioprinting.

PubMed

Park, Ju Young; Choi, Jong-Cheol; Shim, Jin-Hyung; Lee, Jung-Seob; Park, Hyoungjun; Kim, Sung Won; Doh, Junsang; Cho, Dong-Woo

2014-09-01

Bioprinting is a promising technique for engineering composite tissues, such as osteochondral tissues. In this study, as a first step toward bioprinting-based osteochondral tissue regeneration, we systematically examined the behavior of chondrocytes and osteoblasts to hyaluronic acid (HA) and type I collagen (Col-1) hydrogels. First, we demonstrated that cells on hydrogels that were comprised of major native tissue extracellular matrix (ECM) components (i.e. chondrocytes on HA hydrogels and osteoblasts on Col-1 hydrogels) exhibited better proliferation and cell function than cells on non-native ECM hydrogels (i.e., chondrocytes on Col-1 hydrogels and osteoblasts on HA hydrogels). In addition, cells located near their native ECM hydrogels migrated towards them. Finally, we bioprinted three-dimensional (3D) osteochondral tissue-mimetic structures composed of two compartments, osteoblast-encapsulated Col-1 hydrogels and chondrocyte-encapsulated HA hydrogels, and found viability and functions of each cell type were well maintained within the 3D structures up to 14 days in vitro. These results suggest that with proper choice of hydrogel materials, bioprinting-based approaches can be successfully applied for osteochondral tissue regeneration.

Cadmium sulfide quantum dots/poly(acrylic acid-co-acrylic amide) composite hydrogel synthesized by gamma irradiation

NASA Astrophysics Data System (ADS)

Yang, Tao; Li, Qing; Wen, Wanxin; Hu, Liang; He, Weiwei; Liu, Hanzhou

2018-04-01

To improve the durability and stability of quantum dots (QDs) in the composite hydrogel, an irradiation induced reduction and polymerization-crosslinking method was reported herein where CdS QDs could be synthesized in situ and fastened to polymer chains due to the coordination forces between amino groups and CdS nanoparticles. The morphology and photoluminescence (PL) property of the composite hydrogel were studied. The result indicated that the CdS QDs with uniform size were dispersed evenly in the composite hydrogel, and the introduced CdS QDs had no obvious effect on the hydrogel structure. With the increases of reagent concentrations, PL intensity of the composite hydrogel was enhanced; however, the emission wavelength had no change.

Preparation, optimization and property of PVA-HA/PAA composite hydrogel.

PubMed

Chen, Kai; Liu, Jinlong; Yang, Xuehui; Zhang, Dekun

2017-09-01

PVA-HA/PAA composite hydrogel is prepared by freezing-thawing, PEG dehydration and annealing method. Orthogonal design method is used to choose the optimization combination. Results showed that HA and PVA have the maximum effect on water content. PVA and freezing-thawing cycles have the maximum effect on creep resistance and stress relaxation rate of hydrogel. Annealing temperature and freezing-thawing cycles have the maximum effect on compressive elastic modulus of hydrogel. Comparing with the water content and mechanical properties of 16 kinds of combination, PVA-HA/PAA composite hydrogel with freezing-thawing cycles of 3, annealing temperature of 120°C, PVA of 16%, HA of 2%, PAA of 4% has the optimization comprehensive properties. PVA-HA/PAA composite hydrogel has a porous network structure. There are some interactions between PVA, HA and PAA in hydrogel and the properties of hydrogel are strengthened. The annealing treatment improves the crystalline and crosslinking of hydrogel. Therefore, the annealing PVA-HA/PAA composite hydrogel has good thermostability, strength and mechanical properties. It also has good lubrication property and its friction coefficient is relative low. Copyright © 2017 Elsevier B.V. All rights reserved.

Synthesis of linear low-density polyethylene-g-poly (acrylic acid)-co-starch/organo-montmorillonite hydrogel composite as an adsorbent for removal of Pb(ΙΙ) from aqueous solutions.

PubMed

Irani, Maryam; Ismail, Hanafi; Ahmad, Zulkifli; Fan, Maohong

2015-01-01

The purpose of this work is to remove Pb(II) from the aqueous solution using a type of hydrogel composite. A hydrogel composite consisting of waste linear low density polyethylene, acrylic acid, starch, and organo-montmorillonite was prepared through emulsion polymerization method. Fourier transform infrared spectroscopy (FTIR), Solid carbon nuclear magnetic resonance spectroscopy (CNMR)), silicon(-29) nuclear magnetic resonance spectroscopy (Si NMR)), and X-ray diffraction spectroscope ((XRD) were applied to characterize the hydrogel composite. The hydrogel composite was then employed as an adsorbent for the removal of Pb(II) from the aqueous solution. The Pb(II)-loaded hydrogel composite was characterized using Fourier transform infrared spectroscopy (FTIR)), scanning electron microscopy (SEM)), and X-ray photoelectron spectroscopy ((XPS)). From XPS results, it was found that the carboxyl and hydroxyl groups of the hydrogel composite participated in the removal of Pb(II). Kinetic studies indicated that the adsorption of Pb(II) followed the pseudo-second-order equation. It was also found that the Langmuir model described the adsorption isotherm better than the Freundlich isotherm. The maximum removal capacity of the hydrogel composite for Pb(II) ions was 430mg/g. Thus, the waste linear low-density polyethylene-g-poly (acrylic acid)-co-starch/organo-montmorillonite hydrogel composite could be a promising Pb(II) adsorbent. Copyright © 2014. Published by Elsevier B.V.

Introduction to cell–hydrogel mechanosensing

PubMed Central

Ahearne, Mark

2014-01-01

The development of hydrogel-based biomaterials represents a promising approach to generating new strategies for tissue engineering and regenerative medicine. In order to develop more sophisticated cell-seeded hydrogel constructs, it is important to understand how cells mechanically interact with hydrogels. In this paper, we review the mechanisms by which cells remodel hydrogels, the influence that the hydrogel mechanical and structural properties have on cell behaviour and the role of mechanical stimulation in cell-seeded hydrogels. Cell-mediated remodelling of hydrogels is directed by several cellular processes, including adhesion, migration, contraction, degradation and extracellular matrix deposition. Variations in hydrogel stiffness, density, composition, orientation and viscoelastic characteristics all affect cell activity and phenotype. The application of mechanical force on cells encapsulated in hydrogels can also instigate changes in cell behaviour. By improving our understanding of cell–material mechano-interactions in hydrogels, this should enable a new generation of regenerative medical therapies to be developed. PMID:24748951

Preparation and mechanical characterization of a PNIPA hydrogel composite.

PubMed

Liu, Kaifeng; Ovaert, Timothy C; Mason, James J

2008-04-01

A poly (N-isopropylacrylamide) (PNIPA) hydrogel was synthesized by free radical polymerization and reinforced with a polyurethane foam to make a hydrogel composite. The temperature dependence of the elastic modulus of the PNIPA hydrogel and the composite due to volume phase transition was found using a uniaxial compression test, and the swelling property was investigated using an equilibrium swelling ratio experiment. The gel composite preserves the ability to undergo the volume phase transition and its elastic modulus has strong temperature dependence. The temperature dependence of the elastic modulus and swelling ratio of the gel composite were compared to the PNIPA hydrogel. Not surprisingly, the modulus and swelling ratio of the composite were less dramatic than in the gel.

A novel gene delivery composite system based on biodegradable folate-poly (ester amine) polymer and thermosensitive hydrogel for sustained gene release

PubMed Central

Yang, Yi; Zhao, Hang; Jia, YanPeng; Guo, QingFa; Qu, Ying; Su, Jing; Lu, XiaoLing; Zhao, YongXiang; Qian, ZhiYong

2016-01-01

Local anti-oncogene delivery providing high local concentration of gene, increasing antitumor effect and decreasing systemic side effects is currently attracting interest in cancer therapy. In this paper, a novel local sustained anti-oncogene delivery system, PECE thermoresponsive hydrogel containing folate-poly (ester amine) (FA-PEA) polymer/DNA (tumor suppressor) complexes, is demonstrated. First, a tumor-targeted biodegradable folate-poly (ester amine) (FA-PEA) polymer based on low-molecular-weight polyethyleneimine (PEI) was synthesized and characterized, and the application for targeted gene delivery was investigated. The polymer had slight cytotoxicity and high transfection efficiency in vitro compared with PEI 25k, which indicated that FA-PEA was a potential vector for targeted gene delivery. Meanwhile, we successfully prepared a thermoresponsive PECE hydrogel composite containing FA-PEA/DNA complexes which could contain the genes and slowly release the genes into cells. We concluded the folate-poly (ester amine) (FA-PEA) polymer would be useful for targeted gene delivery, and the novel gene delivery composite based on biodegradable folate-poly (ester amine) polymer and thermosensitive PECE hydrogel showed potential for sustained gene release. PMID:26883682

Novel injectable, self-gelling hydrogel-microparticle composites for bone regeneration consisting of gellan gum and calcium and magnesium carbonate microparticles.

PubMed

Douglas, Timothy E L; Łapa, Agata; Reczyńska, Katarzyna; Krok-Borkowicz, Małgorzata; Pietryga, Krzysztof; Samal, Sangram Keshari; Declercq, Heidi A; Schaubroeck, David; Boone, Marijn; Van der Voort, Pascal; De Schamphelaere, Karel; Stevens, Christian V; Bliznuk, Vitaliy; Balcaen, Lieve; Parakhonskiy, Bogdan V; Vanhaecke, Frank; Cnudde, Veerle; Pamuła, Elżbieta; Skirtach, Andre G

2016-11-21

The suitability of hydrogel biomaterials for bone regeneration can be improved by incorporation of an inorganic phase in particle form, thus maintaining hydrogel injectability. In this study, carbonate microparticles containing different amounts of calcium (Ca) and magnesium (Mg) were added to solutions of the anionic polysaccharide gellan gum (GG) to crosslink GG by release of Ca 2+ and Mg 2+ from microparticles and thereby induce formation of hydrogel-microparticle composites. It was hypothesized that increasing Mg content of microparticles would promote GG hydrogel formation. The effect of Mg incorporation on cytocompatibility and cell growth was also studied. Microparticles were formed by mixing Ca 2+ and Mg 2+ and [Formula: see text] ions in varying concentrations. Microparticles were characterized physiochemically and subsequently mixed with GG solution to form hydrogel-microparticle composites. The elemental Ca:Mg ratio in the mineral formed was similar to the Ca:Mg ratio of the ions added. In the absence of Mg, vaterite was formed. At low Mg content, magnesian calcite was formed. Increasing the Mg content further caused formation of amorphous mineral. Microparticles of vaterite and magnesium calcite did not induce GG hydrogel formation, but addition of Mg-richer amorphous microparticles induced gelation within 20 min. Microparticles were dispersed homogeneously in hydrogels. MG-63 osteoblast-like cells were cultured in eluate from hydrogel-microparticle composites and on the composites themselves. All composites were cytocompatible. Cell growth was highest on composites containing particles with an equimolar Ca:Mg ratio. In summary, carbonate microparticles containing a sufficient amount of Mg induced GG hydrogel formation, resulting in injectable, cytocompatible hydrogel-microparticle composites.

Carbon Nanotubes Reinforced Maleic Anhydride-Modified Xylan-g-Poly(N-isopropylacrylamide) Hydrogel with Multifunctional Properties

PubMed Central

Liu, Xinxin; Song, Tao; Chang, Minmin; Meng, Ling; Wang, Xiaohui; Sun, Runcang; Ren, Junli

2018-01-01

Introducing multifunctional groups and inorganic material imparts xylan-based hydrogels with excellent properties, such as responsiveness to pH, temperature, light, and external magnetic field. In this work, a composite hydrogel was synthesized by introducing acid treated carbon nanotubes (AT-CNTs) into the maleic anhydride modified xylan grafted with poly(N-isopropylacrylamide) (MAX-g-PNIPAM) hydrogels network. It was found that the addition of AT-CNTs affected the MAX-g-PNIPAM hydrogel structure, the swelling ratio and mechanical properties, and imparted the hydrogel with new properties of electrical conductivity and near infrared region (NIR) photothermal conversion. AT-CNTs could reinforce the mechanical properties of MAX-g-PNIPAM hydrogels, being up to 83 kPa for the compressive strength when the amount was 11 wt %, which was eight times than that of PNIPAM hydrogel and four times than that of MAX-g-PNIPAM hydrogel. The electroconductibility was enhanced by the increase of AT-CNTs amounts. Meanwhile, the composite hydrogel also exhibited multiple shape memory and NIR photothermal conversion properties, and water temperature was increased from 26 °C to 56 °C within 8 min under the NIR irradiation. Thus, the AT-CNTs reinforced MAX-g-PNIPAM hydrogel possessed promising multifunctional properties, which offered many potential applications in the fields of biosensors, thermal-arrest technology, and drug-controlled release. PMID:29495611

Carbon Nanotubes Reinforced Maleic Anhydride-Modified Xylan-g-Poly(N-isopropylacrylamide) Hydrogel with Multifunctional Properties.

PubMed

Liu, Xinxin; Song, Tao; Chang, Minmin; Meng, Ling; Wang, Xiaohui; Sun, Runcang; Ren, Junli

2018-02-28

Introducing multifunctional groups and inorganic material imparts xylan-based hydrogels with excellent properties, such as responsiveness to pH, temperature, light, and external magnetic field. In this work, a composite hydrogel was synthesized by introducing acid treated carbon nanotubes (AT-CNTs) into the maleic anhydride modified xylan grafted with poly(N-isopropylacrylamide) (MAX-g-PNIPAM) hydrogels network. It was found that the addition of AT-CNTs affected the MAX-g-PNIPAM hydrogel structure, the swelling ratio and mechanical properties, and imparted the hydrogel with new properties of electrical conductivity and near infrared region (NIR) photothermal conversion. AT-CNTs could reinforce the mechanical properties of MAX-g-PNIPAM hydrogels, being up to 83 kPa for the compressive strength when the amount was 11 wt %, which was eight times than that of PNIPAM hydrogel and four times than that of MAX-g-PNIPAM hydrogel. The electroconductibility was enhanced by the increase of AT-CNTs amounts. Meanwhile, the composite hydrogel also exhibited multiple shape memory and NIR photothermal conversion properties, and water temperature was increased from 26 °C to 56 °C within 8 min under the NIR irradiation. Thus, the AT-CNTs reinforced MAX-g-PNIPAM hydrogel possessed promising multifunctional properties, which offered many potential applications in the fields of biosensors, thermal-arrest technology, and drug-controlled release.

DNA nanotechnology-based composite-type gold nanoparticle-immunostimulatory DNA hydrogel for tumor photothermal immunotherapy.

PubMed

Yata, Tomoya; Takahashi, Yuki; Tan, Mengmeng; Nakatsuji, Hirotaka; Ohtsuki, Shozo; Murakami, Tatsuya; Imahori, Hiroshi; Umeki, Yuka; Shiomi, Tomoki; Takakura, Yoshinobu; Nishikawa, Makiya

2017-11-01

Success of tumor photothermal immunotherapy requires a system that induces heat stress in cancer cells and enhances strong anti-tumor immune responses. Here, we designed a composite-type immunostimulatory DNA hydrogel consisting of a hexapod-like structured DNA (hexapodna) with CpG sequences and gold nanoparticles. Mixing of the properly designed hexapodna and oligodeoxynucleotide-modified gold nanoparticles resulted in the formation of composite-type gold nanoparticle-DNA hydrogels. Laser irradiation of the hydrogel resulted in the release of hexapodna, which efficiently stimulated immune cells to release proinflammatory cytokines. Then, EG7-OVA tumor-bearing mice received an intratumoral injection of a gold nanoparticle-DNA hydrogel, followed by laser irradiation at 780 nm. This treatment increased the local temperature and the mRNA expression of heat shock protein 70 in the tumor tissue, increased tumor-associated antigen-specific IgG levels in the serum, and induced tumor-associated antigen-specific interferon-γ production from splenocytes. Moreover, the treatment significantly retarded the tumor growth and extended the survival of the tumor-bearing mice. Copyright © 2017 Elsevier Ltd. All rights reserved.

Evaluation of wound healing potential of β-chitin hydrogel/nano zinc oxide composite bandage.

PubMed

P T, Sudheesh Kumar; Lakshmanan, Vinoth-Kumar; Raj, Mincy; Biswas, Raja; Hiroshi, Tamura; Nair, Shantikumar V; Jayakumar, Rangasamy

2013-02-01

β-chitin hydrogel/nZnO composite bandage was fabricated and evaluated in detail as an alternative to existing bandages. β-chitin hydrogel was synthesized by dissolving β-chitin powder in Methanol/CaCl(2) solvent, followed by the addition of distilled water. ZnO nanoparticles were added to the β-chitin hydrogel and stirred for homogenized distribution. The resultant slurry was frozen at 0°C for 12 h. The frozen samples were lyophilized for 24 h to obtain porous composite bandages. The bandages showed controlled swelling and degradation. The composite bandages showed blood clotting ability as well as platelet activation, which was higher when compared to the control. The antibacterial activity of the bandages were proven against Staphylococcus aureus (S. aureus) and Escherichia coli (E.coli). Cytocompatibility of the composite bandages were assessed using human dermal fibroblast cells (HDF) and these cells on the composite bandages were viable similar to the Kaltostat control bandages and bare β-chitin hydrogel based bandages. The viability was reduced to 50-60% in bandages with higher concentration of zinc oxide nanoparticles (nZnO) and showed 80-90% viability with lower concentration of nZnO. In vivo evaluation in Sprague Dawley rats (S.D. rats) showed faster healing and higher collagen deposition ability of composite bandages when compared to the control. The prepared bandages can be used on various types of infected wounds with large volume of exudates.

3D-Hydrogel Based Polymeric Nanoreactors for Silver Nano-Antimicrobial Composites Generation.

PubMed

Soto-Quintero, Albanelly; Romo-Uribe, Ángel; Bermúdez-Morales, Víctor H; Quijada-Garrido, Isabel; Guarrotxena, Nekane

2017-08-01

This study underscores the development of Ag hydrogel nanocomposites, as smart substrates for antibacterial uses, via innovative in situ reactive and reduction pathways. To this end, two different synthetic strategies were used. Firstly thiol-acrylate (PSA) based hydrogels were attained via thiol-ene and radical polymerization of polyethylene glycol (PEG) and polycaprolactone (PCL). As a second approach, polyurethane (PU) based hydrogels were achieved by condensation polymerization from diisocyanates and PCL and PEG diols. In fact, these syntheses rendered active three-dimensional (3D) hydrogel matrices which were used as nanoreactors for in situ reduction of AgNO₃ to silver nanoparticles. A redox chemistry of stannous catalyst in PU hydrogel yielded spherical AgNPs formation, even at 4 °C in the absence of external reductant; and an appropriate thiol-functionalized polymeric network promoted spherical AgNPs well dispersed through PSA hydrogel network, after heating up the swollen hydrogel at 103 °C in the presence of citrate-reductant. Optical and swelling behaviors of both series of hydrogel nanocomposites were investigated as key factors involved in their antimicrobial efficacy over time. Lastly, in vitro antibacterial activity of Ag loaded hydrogels exposed to Pseudomona aeruginosa and Escherichia coli strains indicated a noticeable sustained inhibitory effect, especially for Ag-PU hydrogel nanocomposites with bacterial inhibition growth capabilities up to 120 h cultivation.

A novel multi-responsive polyampholyte composite hydrogel with excellent mechanical strength and rapid shrinking rate.

PubMed

Xu, Kun; Tan, Ying; Chen, Qiang; An, Huiyong; Li, Wenbo; Dong, Lisong; Wang, Pixin

2010-05-15

Series of hydrophilic core-shell microgels with cross-linked poly(N-isopropylacrylamide) (PNIPAAm) as core and poly(vinyl amine) (PVAm) as shell are synthesized via surfactant-free emulsion polymerization. Then, the microgels are treated with a small amount of potassium persulfate (KPS) to generate free radicals on the amine nitrogens of PVAm, which subsequently initiate the graft copolymerization of acrylic acid (AA), acryloyloxyethyl trimethyl ammonium chloride (DAC), and acrylamide (AAm) onto microgels to prepare multi-responsive composite hydrogels. The composite hydrogels consist of cross-linked ungrafted polyampholyte chains as the first network and microgels with grafted polyampholyte chains as graft point and second network and show surprising mechanical strength and rapid response rate. The investigation shows the compress strength of composite hydrogels is up to 17-30 MPa, which is 60-100 times higher than that of the hydrogel matrix. The composite hydrogel shows reversible switch of transmittance when traveling the lowest critical temperature (LCST) of microgels. When the composite hydrogel swollen in pH 2.86 solution at ambient condition is immersed into the pH 7.00 solution at 45 °C, a rapid dynamic shrinking can be observed. And the character time (τ) of shrinking dynamic of composite hydrogel is 251.9 min, which is less than that of hydrogel matrix (τ=2273.7 min). Copyright © 2010 Elsevier Inc. All rights reserved.

Poroelastic Mechanical Effects of Hemicelluloses on Cellulosic Hydrogels under Compression

PubMed Central

Lopez-Sanchez, Patricia; Cersosimo, Julie; Wang, Dongjie; Flanagan, Bernadine; Stokes, Jason R.; Gidley, Michael J.

2015-01-01

Hemicelluloses exhibit a range of interactions with cellulose, the mechanical consequences of which in plant cell walls are incompletely understood. We report the mechanical properties of cell wall analogues based on cellulose hydrogels to elucidate the contribution of xyloglucan or arabinoxylan as examples of two hemicelluloses displaying different interactions with cellulose. We subjected the hydrogels to mechanical pressures to emulate the compressive stresses experienced by cell walls in planta. Our results revealed that the presence of either hemicellulose increased the resistance to compression at fast strain rates. However, at slow strain rates, only xyloglucan increased composite strength. This behaviour could be explained considering the microstructure and the flow of water through the composites confirming their poroelastic nature. In contrast, small deformation oscillatory rheology showed that only xyloglucan decreased the elastic moduli. These results provide evidence for contrasting roles of different hemicelluloses in plant cell wall mechanics and man-made cellulose-based composite materials. PMID:25794048

Poroelastic mechanical effects of hemicelluloses on cellulosic hydrogels under compression.

PubMed

Lopez-Sanchez, Patricia; Cersosimo, Julie; Wang, Dongjie; Flanagan, Bernadine; Stokes, Jason R; Gidley, Michael J

2015-01-01

Hemicelluloses exhibit a range of interactions with cellulose, the mechanical consequences of which in plant cell walls are incompletely understood. We report the mechanical properties of cell wall analogues based on cellulose hydrogels to elucidate the contribution of xyloglucan or arabinoxylan as examples of two hemicelluloses displaying different interactions with cellulose. We subjected the hydrogels to mechanical pressures to emulate the compressive stresses experienced by cell walls in planta. Our results revealed that the presence of either hemicellulose increased the resistance to compression at fast strain rates. However, at slow strain rates, only xyloglucan increased composite strength. This behaviour could be explained considering the microstructure and the flow of water through the composites confirming their poroelastic nature. In contrast, small deformation oscillatory rheology showed that only xyloglucan decreased the elastic moduli. These results provide evidence for contrasting roles of different hemicelluloses in plant cell wall mechanics and man-made cellulose-based composite materials.

P25-graphene hydrogels: room-temperature synthesis and application for removal of methylene blue from aqueous solution.

PubMed

Hou, Chengyi; Zhang, Qinghong; Li, Yaogang; Wang, Hongzhi

2012-02-29

Herein we report a room-temperature synthesis of chemically bonded TiO2 (P25)-graphene composite hydrogels and their use as high performance visible light photocatalysts. The three-dimensional (3D) TiO2-carbon composite exhibits a significant enhancement in the reaction rate in the decontamination of methylene blue, compared to the bare P25. The 3D P25-graphene hydrogel is much easier to prepare and apply as a macroscopic device, compared to the 2D P25-graphene sheets. This work could provide new insights into the room-temperature synthesis of graphene-based materials. As a kind of the novel 3D graphene-based composite, the obtained high performance P25-graphene gel could be widely used in the environmental protection issues. Copyright © 2012. Published by Elsevier B.V.

Biocompatible nanomaterials based on dendrimers, hydrogels and hydrogel nanocomposites for use in biomedicine

NASA Astrophysics Data System (ADS)

Khoa Nguyen, Cuu; Quyen Tran, Ngoc; Phuong Nguyen, Thi; Hai Nguyen, Dai

2017-03-01

Over the past decades, biopolymer-based nanomaterials have been developed to overcome the limitations of other macro- and micro- synthetic materials as well as the ever increasing demand for the new materials in nanotechnology, biotechnology, biomedicine and others. Owning to their high stability, biodegradability, low toxicity, and biocompatibility, biopolymer-based nanomaterials hold great promise for various biomedical applications. The pursuit of this review is to briefly describe our recent studies regarding biocompatible biopolymer-based nanomaterials, particularly in the form of dendrimers, hydrogels, and hydrogel composites along with the synthetic and modification approaches for the utilization in drug delivery, tissue engineering, and biomedical implants. Moreover, in vitro and in vivo studies for the toxicity evaluation are also discussed.

A facile and efficient strategy for the fabrication of porous linseed gum/cellulose superabsorbent hydrogels for water conservation.

PubMed

Zhang, Hao; Luan, Qian; Huang, Qingde; Tang, Hu; Huang, Fenghong; Li, Wenlin; Wan, Chuyun; Liu, Changsheng; Xu, Jiqu; Guo, Pingmei; Zhou, Qi

2017-02-10

The linseed gum/cellulose composite hydrogels were successfully fabricated by mixing cellulose and linseed gum solutions dissolved in the NaOH/urea aqueous system and cross-linked with epichlorohydrin. The morphology and structure of the composite hydrogels were investigated by scanning electron microscopy (SEM), Fourier transform infrared (FTIR) spectroscopy, X-ray diffractometry (XRD) and thermogravimetric analysis (TGA). The swelling ratio and water retention properties were investigated. The results revealed that linseed gum mainly contributed to water adsorption, whereas the cellulose acted as a backbone to strengthen the porous structure. This work provided a simple way to prepare cellulose-based superabsorbent hydrogels, which could be potentially applied as an effective water conservation material in agriculture. Copyright © 2016 Elsevier Ltd. All rights reserved.

Silk protein-based hydrogels: Promising advanced materials for biomedical applications.

PubMed

Kapoor, Sonia; Kundu, Subhas C

2016-02-01

Hydrogels are a class of advanced material forms that closely mimic properties of the soft biological tissues. Several polymers have been explored for preparing hydrogels with structural and functional features resembling that of the extracellular matrix. Favourable material properties, biocompatibility and easy processing of silk protein fibers into several forms make it a suitable material for biomedical applications. Hydrogels made from silk proteins have shown a potential in overcoming limitations of hydrogels prepared from conventional polymers. A great deal of effort has been made to control the properties and to integrate novel topographical and functional characteristics in the hydrogel composed from silk proteins. This review provides overview of the advances in silk protein-based hydrogels with a primary emphasis on hydrogels of fibroin. It describes the approaches used to fabricate fibroin hydrogels. Attempts to improve the existing properties or to incorporate new features in the hydrogels by making composites and by improving fibroin properties by genetic engineering approaches are also described. Applications of the fibroin hydrogels in the realms of tissue engineering and controlled release are reviewed and their future potentials are discussed. This review describes the potentiality of silk fibroin hydrogel. Silk Fibroin has been widely recognized as an interesting biomaterial. Due to its properties including high mechanical strength and excellent biocompatibility, it has gained wide attention. Several groups are exploring silk-based materials including films, hydrogels, nanofibers and nanoparticles for different biomedical applications. Although there is a good amount of literature available on general properties and applications of silk based biomaterials, there is an inadequacy of extensive review articles that specifically focus on silk based hydrogels. Silk-based hydrogels have a strong potential to be utilized in biomedical applications. Our work is an effort to highlight the research that has been done in the area of silk-based hydrogels. It aims to provide an overview of the advances that have been made and the future course available. It will provide an overview of the silk-based hydrogels as well as may direct the readers to the specific areas of application. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Magnetic hydrogel nanocomposites and composite nanoparticles--a review of recent patented works.

PubMed

Daniel-da-Silva, Ana L; Carvalho, Rui S; Trindade, Tito

2013-06-01

Magnetic hydrogel nanocomposites and composite nanoparticles form a class of soft materials with remote controllable properties that have attracted great attention due to their potential use in diverse applications. These include medical applications such as controlled drug delivery, clinical imaging and cancer hyperthermia and ecological applications as well, such as wastewater treatment. The present review provides an overview of the patents disclosed and research work developed in the last decade on magnetic hydrogel nanocomposites and magnetic hydrogel composite nanoparticles envisaging the above mentioned applications. In this context, recent patented advances on chemical methods for the preparation of bulk hydrogel nanocomposites and composite nanoparticles will be reviewed.

Cell-laden hydrogels for osteochondral and cartilage tissue engineering.

PubMed

Yang, Jingzhou; Zhang, Yu Shrike; Yue, Kan; Khademhosseini, Ali

2017-07-15

Despite tremendous advances in the field of regenerative medicine, it still remains challenging to repair the osteochondral interface and full-thickness articular cartilage defects. This inefficiency largely originates from the lack of appropriate tissue-engineered artificial matrices that can replace the damaged regions and promote tissue regeneration. Hydrogels are emerging as a promising class of biomaterials for both soft and hard tissue regeneration. Many critical properties of hydrogels, such as mechanical stiffness, elasticity, water content, bioactivity, and degradation, can be rationally designed and conveniently tuned by proper selection of the material and chemistry. Particularly, advances in the development of cell-laden hydrogels have opened up new possibilities for cell therapy. In this article, we describe the problems encountered in this field and review recent progress in designing cell-hydrogel hybrid constructs for promoting the reestablishment of osteochondral/cartilage tissues. Our focus centers on the effects of hydrogel type, cell type, and growth factor delivery on achieving efficient chondrogenesis and osteogenesis. We give our perspective on developing next-generation matrices with improved physical and biological properties for osteochondral/cartilage tissue engineering. We also highlight recent advances in biomanufacturing technologies (e.g. molding, bioprinting, and assembly) for fabrication of hydrogel-based osteochondral and cartilage constructs with complex compositions and microarchitectures to mimic their native counterparts. Despite tremendous advances in the field of regenerative medicine, it still remains challenging to repair the osteochondral interface and full-thickness articular cartilage defects. This inefficiency largely originates from the lack of appropriate tissue-engineered biomaterials that replace the damaged regions and promote tissue regeneration. Cell-laden hydrogel systems have emerged as a promising tissue-engineering platform to address this issue. In this article, we describe the fundamental problems encountered in this field and review recent progress in designing cell-hydrogel constructs for promoting the reestablishment of osteochondral/cartilage tissues. Our focus centers on the effects of hydrogel composition, cell type, and growth factor delivery on achieving efficient chondrogenesis and osteogenesis. We give our perspective on developing next-generation hydrogel/inorganic particle/stem cell hybrid composites with improved physical and biological properties for osteochondral/cartilage tissue engineering. We also highlight recent advances in biomanufacturing and bioengineering technologies (e.g. 3D bioprinting) for fabrication of hydrogel-based osteochondral and cartilage constructs. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Mechanical characteristics of beta sheet-forming peptide hydrogels are dependent on peptide sequence, concentration and buffer composition

PubMed Central

Müller, Michael; König, Finja; Meyer, Nina; Gattlen, Jasmin; Pieles, Uwe; Peters, Kirsten; Kreikemeyer, Bernd; Mathes, Stephanie; Saxer, Sina

2018-01-01

Self-assembling peptide hydrogels can be modified regarding their biodegradability, their chemical and mechanical properties and their nanofibrillar structure. Thus, self-assembling peptide hydrogels might be suitable scaffolds for regenerative therapies and tissue engineering. Owing to the use of various peptide concentrations and buffer compositions, the self-assembling peptide hydrogels might be influenced regarding their mechanical characteristics. Therefore, the mechanical properties and stability of a set of self-assembling peptide hydrogels, consisting of 11 amino acids, made from four beta sheet self-assembling peptides in various peptide concentrations and buffer compositions were studied. The formed self-assembling peptide hydrogels exhibited stiffnesses ranging from 0.6 to 205 kPa. The hydrogel stiffness was mostly affected by peptide sequence followed by peptide concentration and buffer composition. All self-assembling peptide hydrogels examined provided a nanofibrillar network formation. A maximum self-assembling peptide hydrogel dissolution of 20% was observed for different buffer solutions after 7 days. The stability regarding enzymatic and bacterial digestion showed less degradation in comparison to the self-assembling peptide hydrogel dissolution rate in buffer. The tested set of self-assembling peptide hydrogels were able to form stable scaffolds and provided a broad spectrum of tissue-specific stiffnesses that are suitable for a regenerative therapy. PMID:29657766

Bio-inspired self-healing structural color hydrogel

PubMed Central

Fu, Fanfan; Chen, Zhuoyue; Zhao, Ze; Wang, Huan; Shang, Luoran; Gu, Zhongze

2017-01-01

Biologically inspired self-healing structural color hydrogels were developed by adding a glucose oxidase (GOX)- and catalase (CAT)-filled glutaraldehyde cross-linked BSA hydrogel into methacrylated gelatin (GelMA) inverse opal scaffolds. The composite hydrogel materials with the polymerized GelMA scaffold could maintain the stability of an inverse opal structure and its resultant structural colors, whereas the protein hydrogel filler could impart self-healing capability through the reversible covalent attachment of glutaraldehyde to lysine residues of BSA and enzyme additives. A series of unprecedented structural color materials could be created by assembling and healing the elements of the composite hydrogel. In addition, as both the GelMA and the protein hydrogels were derived from organisms, the composite materials presented high biocompatibility and plasticity. These features of self-healing structural color hydrogels make them excellent functional materials for different applications. PMID:28533368

Novel biodegradable hydrogel sponge containing curcumin and honey for wound healing.

PubMed

Momin, M; Kurhade, S; Khanekar, P; Mhatre, S

2016-06-01

To develop and evaluate a biodegradable superporous hydrogel based wound healing composite of chitosan and alginate incorporated with curcumin and honey. A 3(2) factorial design was adopted to optimise the honey-curcumin hydrogel composite sponge (CHS). Sodium alginate and chitosan were dissolved in deionised water and 1% aqueous acetic acid solution at room temperature, respectively. Ethanolic solution of curcumin was poured into the chitosan solution followed by an addition of sodium alginate solution. In situ polymerisation was carried out by adding acrylamide base components to the polymeric solution of curcumin. Finally, honey was added with slow stirring and a sponge was cast on a glass surface by solvent evaporation at 45ºC. The produced sponge was assessed for swelling capacity, moisture loss, tensile strength, biocompatibility, bioadhesion, biodegradation, drug diffusion and wound healing properties. The morphology of CHS was studied by scanning electron microscopy (SEM). The optimised CHS demonstrated a high swelling capacity (111.05 ± 05%), tensile strength (4323gm/mm(2)), in vitro drug diffusion (75.03 ± 3.59%/20days), bioadhesion (20 ± 0.2mg force) and ability of water vapour transmission. A rapid induction of tissue granulation and re-epithelialisation was observed. Time to complete healing (94.14 ± 1.04% wound contraction) was 7 ± 2 days. This study has shown that honey-curcumin hydrogel composite sponge can be formulated by a simple mixing and in situ polymerisation method. The hydrogel base provided a dry wound bed due to excellent fluid absorption capacity. Chitosan and honey contributed to effective faster wound healing. We recommend further clinical studies of the soft sponge wound healing composite for diabetic foot or pressure ulcers.

3D-Hydrogel Based Polymeric Nanoreactors for Silver Nano-Antimicrobial Composites Generation

PubMed Central

Soto-Quintero, Albanelly; Romo-Uribe, Ángel; Bermúdez-Morales, Víctor H.; Quijada-Garrido, Isabel

2017-01-01

This study underscores the development of Ag hydrogel nanocomposites, as smart substrates for antibacterial uses, via innovative in situ reactive and reduction pathways. To this end, two different synthetic strategies were used. Firstly thiol-acrylate (PSA) based hydrogels were attained via thiol-ene and radical polymerization of polyethylene glycol (PEG) and polycaprolactone (PCL). As a second approach, polyurethane (PU) based hydrogels were achieved by condensation polymerization from diisocyanates and PCL and PEG diols. In fact, these syntheses rendered active three-dimensional (3D) hydrogel matrices which were used as nanoreactors for in situ reduction of AgNO3 to silver nanoparticles. A redox chemistry of stannous catalyst in PU hydrogel yielded spherical AgNPs formation, even at 4 °C in the absence of external reductant; and an appropriate thiol-functionalized polymeric network promoted spherical AgNPs well dispersed through PSA hydrogel network, after heating up the swollen hydrogel at 103 °C in the presence of citrate-reductant. Optical and swelling behaviors of both series of hydrogel nanocomposites were investigated as key factors involved in their antimicrobial efficacy over time. Lastly, in vitro antibacterial activity of Ag loaded hydrogels exposed to Pseudomona aeruginosa and Escherichia coli strains indicated a noticeable sustained inhibitory effect, especially for Ag–PU hydrogel nanocomposites with bacterial inhibition growth capabilities up to 120 h cultivation. PMID:28763050

Electrohydrodynamic direct printing on hydrogel: a novel method to obtain fine fibers

NASA Astrophysics Data System (ADS)

Liu, Yuanyuan; Jiang, Chen; Liu, Yi; Li, Dongdong; Hu, Qingxi

2016-09-01

In this study, we proposed a novel method to obtain fine fibers: electrohydrodynamic (EHD) direct printing PCL on hydrogel. The effects of applied voltage, flow rate, plotting speed, hydrogel viscosity on the EHD direct writing process were investigated to obtain the most appropriate set of process conditions. We also compared the fibers obtained from this method with traditional EHD which deposited on aluminum and ethanol-based collectors. We found that fibers collected on the hydrogel were thinner and exhibited pores on the surface due to the hydrogel's facilitation of organic solvents' volatilization in the PCL fibers, which can benefit the attachment of cells. Besides, in our previous study, we found the freeze-thaw crosslinking process could greatly increase mechanical properties of the hydrogel used in our research, so this integration will not only mimic the composition of ECM which is a composite structure with a combination of fibrous proteins within a gelatinous grounded substance but also improve the mechanical properties of the scaffold. This novel method will broaden the application of EHD technology in the field of tissue engineering and other related areas.

The preparations of novel cellulose/phenylboronic acid composite intelligent bio-hydrogel and its glucose, pH-responsive behaviors.

PubMed

Peng, Huafeng; Ning, Xiaoyu; Wei, Gang; Wang, Shaopeng; Dai, Guoliang; Ju, Anqi

2018-09-01

Novel intelligent cellulose/4-vinyl-phenylboronic acid (VPBA) composite bio-hydrogels with glucose and pH-responsiveness were successfully prepared via electron beam irradiation technology at room temperature. The composites were characterized by Fourier transform infrared spectrum (FT-IR) and X-ray photoelectron spectroscopy (XPS). The electron beam irradiation results in the appearance of carbonyl in the polymerization of 4-ethenyl-phenylboronic acid, grafting and cross linking reaction in composites, and a novel composite hydrogel was formed between the poly-4-ethenyl-phenylboronic acid and cellulose matrix. By means of the incorporation of phenylboronic acid groups, the composite hydrogels with pH and glucose responsive properties was produced, and glucose responsive properties were investigated by the self-regulation of insulin release of composite hydrogel through a serial glucose solution with different concentrations, which is having great potential applications in many fields. Copyright © 2018 Elsevier Ltd. All rights reserved.

Evaluation of fibrin-gelatin hydrogel as biopaper for application in skin bioprinting: An in-vitro study.

PubMed

Hakam, Mohammad Sadjad; Imani, Rana; Abolfathi, Nabiollah; Fakhrzadeh, Hossein; Sharifi, Ali Mohammad

2016-01-01

Recent advances in tissue engineering have led to the development of the concept of bioprinting as an interesting alternative to traditional tissue engineering approaches. Biopaper, a biomimetic hydrogel, is an essential component of the bioprinting process. The aim of this work was to synthesize a biopaper made of fibrin-gelatin hybrid hydrogel for application in skin bioprinting. Different composition percentages of the two biopolymer hydrogels, fibrin-gelatin, have been studied for the construction of the biopaper and were examined in terms of water absorption, biodegradability, glucose absorption, mechanical properties and water vapor transmission. Subsequently, tissue fusion study was performed on prepared 3T3 fibroblast cell line pellets embedded into the hydrogel. Based on the obtained results, fibrin-gelatin blend hydrogel with the same proportion of two components provides a natural scaffold for fibroblast-based bioink embedding and culture. The suggested optimized hydrogel was a suitable candidate as a biopaper for skin bioprinting technology.

Effects of pore forming agents on chitosan-graft-poly(N-vinylpyrrolidone) hydrogel properties for use as a matrix for floating drug delivery

NASA Astrophysics Data System (ADS)

Budianto, E.; Al-Shidqi, M. F.; Cahyana, A. H.

2017-07-01

Eradicating H. pylori-based infection by using conventional oral dosage form of amoxicillin trihydrate finds difficulties to overcome rapid gastric retention time. Encapsulating amoxicillin trihydrate in floating drug delivery system may solve the problem. In this research, the floating drug delivery system of amoxicillin trihydrate encapsulated in floating chitosan-graft-poly(N-vinyl pyrrolidone) hydrogels containing CaCO3 and NaHCO3 as pore forming agents has been successfully prepared. Pore forming agents used was varied with the ratio of 10 to 25% pore forming agents to total mass of the used materials. The hydrogel were characterizedusing FTIR spectrophotometer and stereo microscope. As pore forming agents compositions increased, the porosity (%) and floating properties increased but followed by decrease in drug entrapment efficiency. Most of the floating hydrogels possessed floating ability longer than 180 min and the highest porosity was found in hydrogel containing 25% NaHCO3. Hydrogel containing CaCO3 showed sustained drug release profile than hydrogel containing NaHCO3. However, the optimum formulation was achieved at composition of 10% NaHCO3 with 57% of drug entrapped within the hydrogel and 43% drug released. The results of these studies show that NaHCO3 is an effective pore forming agents for chitosan-graft-poly(N-vinyl pyrrolidone) hydrogel preparation as compare to CaCO3.

Dual-functional transdermal drug delivery system with controllable drug loading based on thermosensitive poloxamer hydrogel for atopic dermatitis treatment

NASA Astrophysics Data System (ADS)

Wang, Wenyi; Wat, Elaine; Hui, Patrick C. L.; Chan, Ben; Ng, Frency S. F.; Kan, Chi-Wai; Wang, Xiaowen; Hu, Huawen; Wong, Eric C. W.; Lau, Clara B. S.; Leung, Ping-Chung

2016-04-01

The treatment of atopic dermatitis (AD) has long been viewed as a problematic issue by the medical profession. Although a wide variety of complementary therapies have been introduced, they fail to combine the skin moisturizing and drug supply for AD patients. This study reports the development of a thermo-sensitive Poloxamer 407/Carboxymethyl cellulose sodium (P407/CMCs) composite hydrogel formulation with twin functions of moisture and drug supply for AD treatment. It was found that the presence of CMCs can appreciably improve the physical properties of P407 hydrogel, which makes it more suitable for tailored drug loading. The fabricated P407/CMCs composite hydrogel was also characterized in terms of surface morphology by field emission scanning electron microscopy (FE-SEM), rheological properties by a rheometer, release profile in vitro by dialysis method and cytotoxicity test. More importantly, the findings from transdermal drug delivery behavior revealed that P407/CMCs showed desirable percutaneous performance. Additionally, analysis of cytotoxicity test suggested that P407/CMCs composite hydrogel is a high-security therapy for clinical trials and thus exhibits a promising way to treat AD with skin moisturizing and medication.

Dual-functional transdermal drug delivery system with controllable drug loading based on thermosensitive poloxamer hydrogel for atopic dermatitis treatment

PubMed Central

Wang, Wenyi; Wat, Elaine; Hui, Patrick C. L.; Chan, Ben; Ng, Frency S. F.; Kan, Chi-Wai; Wang, Xiaowen; Hu, Huawen; Wong, Eric C. W.; Lau, Clara B. S.; Leung, Ping-Chung

2016-01-01

The treatment of atopic dermatitis (AD) has long been viewed as a problematic issue by the medical profession. Although a wide variety of complementary therapies have been introduced, they fail to combine the skin moisturizing and drug supply for AD patients. This study reports the development of a thermo-sensitive Poloxamer 407/Carboxymethyl cellulose sodium (P407/CMCs) composite hydrogel formulation with twin functions of moisture and drug supply for AD treatment. It was found that the presence of CMCs can appreciably improve the physical properties of P407 hydrogel, which makes it more suitable for tailored drug loading. The fabricated P407/CMCs composite hydrogel was also characterized in terms of surface morphology by field emission scanning electron microscopy (FE-SEM), rheological properties by a rheometer, release profile in vitro by dialysis method and cytotoxicity test. More importantly, the findings from transdermal drug delivery behavior revealed that P407/CMCs showed desirable percutaneous performance. Additionally, analysis of cytotoxicity test suggested that P407/CMCs composite hydrogel is a high-security therapy for clinical trials and thus exhibits a promising way to treat AD with skin moisturizing and medication. PMID:27090158

Property-based design: optimization and characterization of polyvinyl alcohol (PVA) hydrogel and PVA-matrix composite for artificial cornea.

PubMed

Jiang, Hong; Zuo, Yi; Zhang, Li; Li, Jidong; Zhang, Aiming; Li, Yubao; Yang, Xiaochao

2014-03-01

Each approach for artificial cornea design is toward the same goal: to develop a material that best mimics the important properties of natural cornea. Accordingly, the selection and optimization of corneal substitute should be based on their physicochemical properties. In this study, three types of polyvinyl alcohol (PVA) hydrogels with different polymerization degree (PVA1799, PVA2499 and PVA2699) were prepared by freeze-thawing techniques. After characterization in terms of transparency, water content, water contact angle, mechanical property, root-mean-square roughness and protein adsorption behavior, the optimized PVA2499 hydrogel with similar properties of natural cornea was selected as a matrix material for artificial cornea. Based on this, a biomimetic artificial cornea was fabricated with core-and-skirt structure: a transparent PVA hydrogel core, surrounding by a ringed PVA-matrix composite skirt that composed of graphite, Fe-doped nano hydroxyapatite (n-Fe-HA) and PVA hydrogel. Different ratio of graphite/n-Fe-HA can tune the skirt color from dark brown to light brown, which well simulates the iris color of Oriental eyes. Moreover, morphologic and mechanical examination showed that an integrated core-and-skirt artificial cornea was formed from an interpenetrating polymer network, no phase separation appeared on the interface between the core and the skirt.

Cationic hemicellulose-based hydrogels for arsenic and chromium removal from aqueous solutions.

PubMed

Dax, Daniel; Chávez, María Soledad; Xu, Chunlin; Willför, Stefan; Mendonça, Regis Teixeira; Sánchez, Julio

2014-10-13

In this work the synthesis of hemicellulose-based hydrogels and their application for the removal of arsenic and chromium ions is described. In a first step O-acetyl galactoglucomannan (GGM) was subjected to a transesterification applying glycidyl methacrylate (GMA) for the synthesis of novel GGM macromonomers. Two distinguished and purified GGM fractions with molar mass of 7.1 and 28 kDa were used as starting materials. The resulting GGM macromonomers (GGM-MA) contained well-defined amounts of methacrylate groups as determined by (1)H NMR spectroscopy. Selected GGM-MA derivatives were consecutively applied as a crosslinker in the synthesis of tailored hydrogels using [2-(methacryloyloxy)ethyl]trimethylammonium chloride (MeDMA) as monomer. The swelling rate of the hydrogels was determined and the coherence between the swelling rate and the hydrogel composition was examined. The morphology of the GGM-based hydrogels was analysed by SEM and the hydrogels revealed a high surface area and were assessed in respect to their ability to remove arsenate and chromate ions from aqueous solutions. The presented bio-based hydrogels are of high interest especially for the mining industries as a sustainable material for the treatment of their highly contaminated wastewaters. Copyright © 2014 Elsevier Ltd. All rights reserved.

Biocompatibility of hydrogel-based scaffolds for tissue engineering applications.

PubMed

Naahidi, Sheva; Jafari, Mousa; Logan, Megan; Wang, Yujie; Yuan, Yongfang; Bae, Hojae; Dixon, Brian; Chen, P

2017-09-01

Recently, understanding of the extracellular matrix (ECM) has expanded rapidly due to the accessibility of cellular and molecular techniques and the growing potential and value for hydrogels in tissue engineering. The fabrication of hydrogel-based cellular scaffolds for the generation of bioengineered tissues has been based on knowledge of the composition and structure of ECM. Attempts at recreating ECM have used either naturally-derived ECM components or synthetic polymers with structural integrity derived from hydrogels. Due to their increasing use, their biocompatibility has been questioned since the use of these biomaterials needs to be effective and safe. It is not surprising then that the evaluation of biocompatibility of these types of biomaterials for regenerative and tissue engineering applications has been expanded from being primarily investigated in a laboratory setting to being applied in the multi-billion dollar medicinal industry. This review will aid in the improvement of design of non-invasive, smart hydrogels that can be utilized for tissue engineering and other biomedical applications. In this review, the biocompatibility of hydrogels and design criteria for fabricating effective scaffolds are examined. Examples of natural and synthetic hydrogels, their biocompatibility and use in tissue engineering are discussed. The merits and clinical complications of hydrogel scaffold use are also reviewed. The article concludes with a future outlook of the field of biocompatibility within the context of hydrogel-based scaffolds. Copyright © 2017 Elsevier Inc. All rights reserved.

Surface-modified silk hydrogel containing hydroxyapatite nanoparticle with hyaluronic acid-dopamine conjugate.

PubMed

Kim, Hyung Hwan; Park, Jong Bo; Kang, Min Ji; Park, Young Hwan

2014-09-01

Silk fibroin/hydroxyapatite (SF/HAp) composite hydrogels were fabricated in this study, having different HAp contents (0-33 wt%) in SF matrix hydrogel. Surface modification of HAp nanoparticle with hyaluronic acid (HA)-dopamine (DA) conjugate improved a dispersibility of HAp in aqueous SF solution due to its negatively charged surface and therefore, fabrication of the SF composite hydrogel having HAp nanoparticles inside could be possible. Zeta potential of surface-modified HAP was examined by ELS. It demonstrates that surface of HAp was well modified to a negative charge with HA-DA. Morphological structure of SF hydrogel containing surface-modified HAp was examined by FE-SEM for analyzing pore structure of hydrogel and deposition of HAp nanoparticle in SF hydrogel. It was found that HAp nanoparticles were uniformly deposited on the pore wall of SF hydrogel. Structural characteristics of SF/HAp composite hydrogel was performed using X-ray diffraction and FT-IR analysis. It was found that β-sheet crystal conformation of SF was significantly influenced by the HAp content during gelation of a mixture of SF and HAp. As a result of MTT assay, the SF/HAp composite hydrogel showed excellent cell proliferation ability. Therefore, it is expected that SF hydrogel containing HAp nanoparticles has a high potential as bone regeneration scaffold. Copyright © 2014 Elsevier B.V. All rights reserved.

Photopolymerizable chitosan-collagen hydrogels for bone tissue engineering.

PubMed

Arakawa, Christopher; Ng, Ronald; Tan, Steven; Kim, Soyon; Wu, Benjamin; Lee, Min

2017-01-01

Photopolymerizable hydrogels derived from naturally occurring polymers have attracted significant interest in tissue-engineering applications due to their excellent biocompatibility, hydrophilic nature favourable for cell ingrowth and ability to be cured in situ through a minimally invasive procedure. In this study, we developed a composite hydrogel consisting of photocrosslinkable methacrylated glycol chitosan (MeGC) and semi-interpenetrating collagen (Col) with a riboflavin photoinitiator under blue light. The incorporation of Col in MeGC hydrogels enhanced the compressive modulus and slowed the degradation rate of the hydrogels. MeGC-Col composite hydrogels significantly enhanced cellular attachment, spreading, proliferation and osteogenic differentiation of mouse bone marrow stromal cells (BMSCs) seeded on the hydrogels compared with pure MeGC hydrogels, as observed by upregulated alkaline phosphatase (ALP) activity as well as increased mineralization. Similarly, when cells were encapsulated within hydrogels, BMSCs exhibited greater proliferation, ALP activity and mineral deposits in the presence of Col. These findings demonstrate that MeGC-Col composite hydrogels may be useful in promoting bone regeneration. Copyright © 2014 John Wiley & Sons, Ltd. Copyright © 2014 John Wiley & Sons, Ltd.

Automation of 3D cell culture using chemically defined hydrogels.

PubMed

Rimann, Markus; Angres, Brigitte; Patocchi-Tenzer, Isabel; Braum, Susanne; Graf-Hausner, Ursula

2014-04-01

Drug development relies on high-throughput screening involving cell-based assays. Most of the assays are still based on cells grown in monolayer rather than in three-dimensional (3D) formats, although cells behave more in vivo-like in 3D. To exemplify the adoption of 3D techniques in drug development, this project investigated the automation of a hydrogel-based 3D cell culture system using a liquid-handling robot. The hydrogel technology used offers high flexibility of gel design due to a modular composition of a polymer network and bioactive components. The cell inert degradation of the gel at the end of the culture period guaranteed the harmless isolation of live cells for further downstream processing. Human colon carcinoma cells HCT-116 were encapsulated and grown in these dextran-based hydrogels, thereby forming 3D multicellular spheroids. Viability and DNA content of the cells were shown to be similar in automated and manually produced hydrogels. Furthermore, cell treatment with toxic Taxol concentrations (100 nM) had the same effect on HCT-116 cell viability in manually and automated hydrogel preparations. Finally, a fully automated dose-response curve with the reference compound Taxol showed the potential of this hydrogel-based 3D cell culture system in advanced drug development.

Novel levan and pNIPA temperature sensitive hydrogels for 5-ASA controlled release.

PubMed

Osman, Asila; Oner, Ebru Toksoy; Eroglu, Mehmet S

2017-06-01

Levan based cross-linker was successfully synthesized and used to prepare a series of more biocompatible and temperature responsive levan/N-isopropyl acrylamide (levan/pNIPA) hydrogels by redox polymerization at room temperature. Volume phase transition temperature (VPTT) of the hydrogels were precisely determined by derivative differential scanning calorimetry (DDSC). Incorporation of levan into the pNIPA hydrogel increased the VPTT from 32.8°C to 35.09°C, approaching to body temperature. Swelling behavior and 5-aminosalicylic acid (5-ASA) release of the hydrogels were found to vary significantly with temperature and composition. Moreover, a remarkable increase in thermal stability of levan within hydrogel with increase of pNIPA content was recorded. The biocompatibility of the hydrogels were tested against mouse fibroblast L929 cell line in phosphate buffer saline (PBS, pH 7.4). The hydrogels showed increasing biocompatibility with increasing levan ratio, indicating levan enhanced the hydrogel surface during swelling. Copyright © 2017 Elsevier Ltd. All rights reserved.

Composite chitosan hydrogels for extended release of hydrophobic drugs.

PubMed

Delmar, Keren; Bianco-Peled, Havazelet

2016-01-20

A composite chitosan hydrogel durable in physiological conditions intended for sustained release of hydrophobic drugs was investigated. The design is based on chitosan crosslinked with genipin with embedded biocompatible non-ionic microemulsion (ME). A prolonged release period of 48 h in water, and of 24h in phosphate buffer saline (PBS) of pH 7.4 was demonstrated for Nile red and curcumin. The differences in release patterns in water and PBS were attributed to distinct dissimilarities in the swelling behaviors; in water, the hydrogels swell enormously, while in PBS they expel water and shrink. The release mechanism dominating this system is complex due to intermolecular bonding between the oil droplets and the polymeric network, as confirmed by Fourier transform infrared spectroscopy (FTIR) experiments. This is the first time that oil in water microemulsions were introduced into a chitosan hydrogels for the creation of a hydrophobic drug delivery system. Copyright © 2015 Elsevier Ltd. All rights reserved.

Double network bacterial cellulose hydrogel to build a biology-device interface.

PubMed

Shi, Zhijun; Li, Ying; Chen, Xiuli; Han, Hongwei; Yang, Guang

2014-01-21

Establishing a biology-device interface might enable the interaction between microelectronics and biotechnology. In this study, electroactive hydrogels have been produced using bacterial cellulose (BC) and conducting polymer (CP) deposited on the BC hydrogel surface to cover the BC fibers. The structures of these composites thus have double networks, one of which is a layer of electroactive hydrogels combined with BC and CP. The electroconductivity provides the composites with capabilities for voltage and current response, and the BC hydrogel layer provides good biocompatibility, biodegradability, bioadhesion and mass transport properties. Such a system might allow selective biological functions such as molecular recognition and specific catalysis and also for probing the detailed genetic and molecular mechanisms of life. A BC-CP composite hydrogel could then lead to a biology-device interface. Cyclic voltammetry and electrochemical impedance spectroscopy (EIS) are used here to study the composite hydrogels' electroactive property. BC-PAni and BC-PPy respond to voltage changes. This provides a mechanism to amplify electrochemical signals for analysis or detection. BC hydrogels were found to be able to support the growth, spreading and migration of human normal skin fibroblasts without causing any cytotoxic effect on the cells in the cell culture. These double network BC-CP hydrogels are biphasic Janus hydrogels which integrate electroactivity with biocompatibility, and might provide a biology-device interface to produce implantable devices for personalized and regenerative medicine.

Double network bacterial cellulose hydrogel to build a biology-device interface

NASA Astrophysics Data System (ADS)

Shi, Zhijun; Li, Ying; Chen, Xiuli; Han, Hongwei; Yang, Guang

2013-12-01

Establishing a biology-device interface might enable the interaction between microelectronics and biotechnology. In this study, electroactive hydrogels have been produced using bacterial cellulose (BC) and conducting polymer (CP) deposited on the BC hydrogel surface to cover the BC fibers. The structures of these composites thus have double networks, one of which is a layer of electroactive hydrogels combined with BC and CP. The electroconductivity provides the composites with capabilities for voltage and current response, and the BC hydrogel layer provides good biocompatibility, biodegradability, bioadhesion and mass transport properties. Such a system might allow selective biological functions such as molecular recognition and specific catalysis and also for probing the detailed genetic and molecular mechanisms of life. A BC-CP composite hydrogel could then lead to a biology-device interface. Cyclic voltammetry and electrochemical impedance spectroscopy (EIS) are used here to study the composite hydrogels' electroactive property. BC-PAni and BC-PPy respond to voltage changes. This provides a mechanism to amplify electrochemical signals for analysis or detection. BC hydrogels were found to be able to support the growth, spreading and migration of human normal skin fibroblasts without causing any cytotoxic effect on the cells in the cell culture. These double network BC-CP hydrogels are biphasic Janus hydrogels which integrate electroactivity with biocompatibility, and might provide a biology-device interface to produce implantable devices for personalized and regenerative medicine.

Creating Stiff, Tough, and Functional Hydrogel Composites with Low-Melting-Point Alloys.

PubMed

Takahashi, Riku; Sun, Tao Lin; Saruwatari, Yoshiyuki; Kurokawa, Takayuki; King, Daniel R; Gong, Jian Ping

2018-04-01

Reinforcing hydrogels with a rigid scaffold is a promising method to greatly expand the mechanical and physical properties of hydrogels. One of the challenges of creating hydrogel composites is the significant stress that occurs due to swelling mismatch between the water-swollen hydrogel matrix and the rigid skeleton in aqueous media. This stress can cause physical deformation (wrinkling, buckling, or fracture), preventing the fabrication of robust composites. Here, a simple yet versatile method is introduced to create "macroscale" hydrogel composites, by utilizing a rigid reinforcing phase that can relieve stress-induced deformation. A low-melting-point alloy that can transform from a load-bearing solid state to a free-deformable liquid state at relatively low temperature is used as a reinforcing skeleton, which enables the release of any swelling mismatch, regardless of the matrix swelling degree in liquid media. This design can generally provide hydrogels with hybridized functions, including excellent mechanical properties, shape memory, and thermal healing, which are often difficult or impossible to achieve with single-component hydrogel systems. Furthermore, this technique enables controlled electrochemical reactions and channel-structure templating in hydrogel matrices. This work may play an important role in the future design of soft robots, wearable electronics, and biocompatible functional materials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enzymatically crosslinked silk-hyaluronic acid hydrogels.

PubMed

Raia, Nicole R; Partlow, Benjamin P; McGill, Meghan; Kimmerling, Erica Palma; Ghezzi, Chiara E; Kaplan, David L

2017-07-01

In this study, silk fibroin and hyaluronic acid (HA) were enzymatically crosslinked to form biocompatible composite hydrogels with tunable mechanical properties similar to that of native tissues. The formation of di-tyrosine crosslinks between silk fibroin proteins via horseradish peroxidase has resulted in a highly elastic hydrogel but exhibits time-dependent stiffening related to silk self-assembly and crystallization. Utilizing the same method of crosslinking, tyramine-substituted HA forms hydrophilic and bioactive hydrogels that tend to have limited mechanics and degrade rapidly. To address the limitations of these singular component scaffolds, HA was covalently crosslinked with silk, forming a composite hydrogel that exhibited both mechanical integrity and hydrophilicity. The composite hydrogels were assessed using unconfined compression and infrared spectroscopy to reveal of the physical properties over time in relation to polymer concentration. In addition, the hydrogels were characterized by enzymatic degradation and for cytotoxicity. Results showed that increasing HA concentration, decreased gelation time, increased degradation rate, and reduced changes that were observed over time in mechanics, water retention, and crystallization. These hydrogel composites provide a biologically relevant system with controllable temporal stiffening and elasticity, thus offering enhanced tunable scaffolds for short or long term applications in tissue engineering. Copyright © 2017 Elsevier Ltd. All rights reserved.

Poly(n-vinylpyrrolidone) hydrogels: 2.Hydrogel composites as wound dressing for tropical environment

NASA Astrophysics Data System (ADS)

Himly, N.; Darwis, D.; Hardiningsih, L.

1993-10-01

POLY(N-VINYLPYRROLIDONE) HYDROGELS: 2. HYDROGEL COMPOSITES AS WOUND DRESSING FOR TROPICAL ENVIRONMENT. The effects of irradiation on hydration and other properties of poly(vinylpyrrolidone) (PVP) hydrogel composites have been investigated. The aqueous solution of vinylpyrrolidone (VP) 10 wt % was mixed with several additives such as agar and polyethylen glycol (PEG). The solution was then irradiated with gamma rays from Cobalt-60 source at room temperature. Several parameters such as elongation at break (EB), tensile strength (TS), degree of swelling (DS), water vapor transmission rate (WVTR), equilibrium water content (EWC), microbial growth and penetration test, and water activity (Aw) were analysed at room temperature of 29 ±2°C humidity of 80 ± 10%. Results show that elongation at break of hydrogel membranes with initial composition of VP with agar, VP with agar and PEG were 240 % and 250 % kGy, the equilibrium water content of membranes were 96 to 90%, whereas degree of swelling were 55 to 10. The WVTR of hydrogel membranes with initial composition of VP with agar and PEG was 70 g m -2h -1, while the water activity was 0.9. Such hydrogel membranes exhibits the following properties: They are elastic, transparent, flexible, impermeable for bacteria. They absopt a high capacity of water, attached to healthy skin but not to the wound and they are easy to remove. These properties of the hydrogel membranes allow for applying as a wound dressings in tropical environment.

Multifunctional hydrogel nano-probes for atomic force microscopy

PubMed Central

Lee, Jae Seol; Song, Jungki; Kim, Seong Oh; Kim, Seokbeom; Lee, Wooju; Jackman, Joshua A.; Kim, Dongchoul; Cho, Nam-Joon; Lee, Jungchul

2016-01-01

Since the invention of the atomic force microscope (AFM) three decades ago, there have been numerous advances in its measurement capabilities. Curiously, throughout these developments, the fundamental nature of the force-sensing probe—the key actuating element—has remained largely unchanged. It is produced by long-established microfabrication etching strategies and typically composed of silicon-based materials. Here, we report a new class of photopolymerizable hydrogel nano-probes that are produced by bottom-up fabrication with compressible replica moulding. The hydrogel probes demonstrate excellent capabilities for AFM imaging and force measurement applications while enabling programmable, multifunctional capabilities based on compositionally adjustable mechanical properties and facile encapsulation of various nanomaterials. Taken together, the simple, fast and affordable manufacturing route and multifunctional capabilities of hydrogel AFM nano-probes highlight the potential of soft matter mechanical transducers in nanotechnology applications. The fabrication scheme can also be readily utilized to prepare hydrogel cantilevers, including in parallel arrays, for nanomechanical sensor devices. PMID:27199165

Research on torsional friction behavior and fluid load support of PVA/HA composite hydrogel.

PubMed

Chen, Kai; Zhang, Dekun; Yang, Xuehui; Cui, Xiaotong; Zhang, Xin; Wang, Qingliang

2016-09-01

Hydrogels have been extensively studied for use as synthetic articular cartilage. This study aimed to investigate (1) the torsional friction contact state and the transformation mechanism of PVA/HA composite hydrogel against CoCrMo femoral head and (2) effects of load and torsional angle on torsional friction behavior. The finite element method was used to study fluid load support of PVA/HA composite hydrogel. Results show fluid loss increases gradually of PVA/HA composite hydrogel with torsional friction time, leading to fluid load support decreases. The contact state changes from full slip state to stick-slip mixed state. As the load increases, friction coefficient and adhesion zone increase gradually. As the torsional angle increases, friction coefficient and slip trend of the contact interface increase, resulting in the increase of the slip zone and the reduction of the adhesion zone. Fluid loss increases of PVA/HA composite hydrogel as the load and the torsional angle increase, which causes the decrease of fluid load support and the increase of friction coefficient. Copyright © 2016 Elsevier Ltd. All rights reserved.

Phase-Separated Polyaniline/Graphene Composite Electrodes for High-Rate Electrochemical Supercapacitors.

PubMed

Wu, Jifeng; Zhang, Qin'e; Zhou, An'an; Huang, Zhifeng; Bai, Hua; Li, Lei

2016-12-01

Polyaniline/graphene hydrogel composites with a macroscopically phase-separated structure are prepared. The composites show high specific capacitance and excellent rate performance. Further investigation demonstrates that polyaniline inside the graphene hydrogel has low rate performance, thus a phase-separated structure, in which polyaniline is mainly outside the graphene hydrogel matrix, can enhance the rate performance of the composites. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nanocellulose-alginate hydrogel for cell encapsulation.

PubMed

Park, Minsung; Lee, Dajung; Hyun, Jinho

2015-02-13

TEMPO-oxidized bacterial cellulose (TOBC)-sodium alginate (SA) composites were prepared to improve the properties of hydrogel for cell encapsulation. TOBC fibers were obtained using a TEMPO/NaBr/NaClO system at pH 10 and room temperature. The fibrillated TOBCs mixed with SA were cross-linked in the presence of Ca(2+) solution to form hydrogel composites. The compression strength and chemical stability of the TOBC/SA composites were increased compared with the SA hydrogel, which indicated that TOBC performed an important function in enhancing the structural, mechanical and chemical stability of the composites. Cells were successfully encapsulated in the TOBC/SA composites, and the viability of cells was investigated. TOBC/SA composites can be a potential candidate for cell encapsulation engineering. Copyright © 2014 Elsevier Ltd. All rights reserved.

Dual-pH/Magnetic-Field-Controlled Drug Delivery Systems Based on Fe3 O4 @SiO2 -Incorporated Salecan Graft Copolymer Composite Hydrogels.

PubMed

Hu, Xinyu; Wang, Yongmei; Zhang, Liangliang; Xu, Man; Zhang, Jianfa; Dong, Wei

2017-10-09

Salecan is a water-soluble extracellular β-glucan and has excellent physicochemical and biological properties for hydrogel preparation. In this study, a new pH/magnetic field dual-responsive hydrogel was prepared by the graft copolymerization of salecan with 4-pentenoic acid (PA) and N-hydroxyethylacrylamide (HEAA) in the presence of Fe 3 O 4 @SiO 2 nanoparticles for doxorubicin hydrochloride (DOX) release. Integration of Fe 3 O 4 @SiO 2 nanoparticles in salecan-g-poly(PA-co-HEAA) copolymers afforded magnetic sensitivity to the original material. DOX-loaded hydrogels exhibited a clear capacity for pH/magnetic field dual-responsive controlled drug release. Lowering the pH to acidic conditions or introducing an external magnetic field caused an enhancement in DOX release. This salecan-g-poly(PA-co-HEAA)/Fe 3 O 4 @SiO 2 composite hydrogel is a promising drug carrier for magnetically targeted drug delivery with enhanced DOX cytotoxicity against A549 cells. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tough Composite Hydrogels with High Loading and Local Release of Biological Drugs.

PubMed

Li, Jianyu; Weber, Eckhard; Guth-Gundel, Sabine; Schuleit, Michael; Kuttler, Andreas; Halleux, Christine; Accart, Nathalie; Doelemeyer, Arno; Basler, Anne; Tigani, Bruno; Wuersch, Kuno; Fornaro, Mara; Kneissel, Michaela; Stafford, Alexander; Freedman, Benjamin R; Mooney, David J

2018-05-01

Hydrogels are under active development for controlled drug delivery, but their clinical translation is limited by low drug loading capacity, deficiencies in mechanical toughness and storage stability, and poor control over the drug release that often results in burst release and short release duration. This work reports a design of composite clay hydrogels, which simultaneously achieve a spectrum of mechanical, storage, and drug loading/releasing properties to address the critical needs from translational perspectives. The clay nanoparticles provide large surface areas to adsorb biological drugs, and assemble into microparticles that are physically trapped within and toughen hydrogel networks. The composite hydrogels demonstrate feasibility of storage, and extended release of large quantities of an insulin-like growth factor-1 mimetic protein (8 mg mL -1 ) over four weeks. The release rate is primarily governed by ionic exchange and can be upregulated by low pH, which is typical for injured tissues. A rodent model of Achilles tendon injury is used to demonstrate that the composite hydrogels allow for highly extended and localized release of biological drugs in vivo, while demonstrating biodegradation and biocompatibility. These attributes make the composite hydrogel a promising system for drug delivery and regenerative medicine. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Gelatin- and starch-based hydrogels. Part B: In vitro mesenchymal stem cell behavior on the hydrogels.

PubMed

Van Nieuwenhove, Ine; Salamon, Achim; Adam, Stefanie; Dubruel, Peter; Van Vlierberghe, Sandra; Peters, Kirsten

2017-04-01

Tissue regeneration often occurs only to a limited extent. By providing a three-dimensional matrix serving as a surrogate extracellular matrix that promotes adult stem cell adhesion, proliferation and differentiation, scaffold-guided tissue regeneration aims at overcoming this limitation. In this study, we applied hydrogels made from crosslinkable gelatin, the hydrolyzed form of collagen, and functionalized starch which were characterized in depth and optimized as described in Van Nieuwenhove et al., 2016. "Gelatin- and Starch-Based Hydrogels. Part A: Hydrogel Development, Characterization and Coating", Carbohydrate Polymers 152:129-39. Collagen is the main structural protein in animal connective tissue and the most abundant protein in mammals. Starch is a carbohydrate consisting of a mixture of amylose and amylopectin. Hydrogels were developed with varying chemical composition (ratio of starch to gelatin applied) and different degrees of methacrylation of the applied gelatin phase. The hydrogels used exhibited no adverse effect on viability of the stem cells cultured on them. Moreover, initial cell adhesion did not differ significantly between them, while the strongest proliferation was observed on the hydrogel with the highest degree of cross-linking. On the least crosslinked and thus most flexible hydrogels, the highest degree of adipogenic differentiation was found, while osteogenic differentiation was the strongest on the most rigid, starch-blended hydrogels. Hydrogel coating with extracellular matrix compounds aggrecan or fibronectin prior to cell seeding exhibited no significant effects. Thus, gelatin-based hydrogels can be optimized regarding maximum promotion of either adipogenic or osteogenic stem cell differentiation in vitro, which makes them promising candidates for in vivo evaluation in clinical studies aiming at either soft or hard tissue regeneration. Copyright © 2017 Elsevier Ltd. All rights reserved.

The osteogenic differentiation of dog bone marrow mesenchymal stem cells in a thermo-sensitive injectable chitosan/collagen/β-glycerophosphate hydrogel: in vitro and in vivo.

PubMed

Sun, Bin; Ma, Wei; Su, Fang; Wang, Yi; Liu, Jiaqiang; Wang, Dongshen; Liu, Hongchen

2011-09-01

Type I collagen was added to the composite chitosan solution in a ratio of 1:2 to build a physical cross-linked self-forming chitosan/collagen/β-GP hydrogel. Osteogenic properties of this novel injectable hydrogel were evaluated. Gelation time was about 8 min which offered enough time for handling a mixture containing cells and the subsequent injection. Scanning electronic microscopy (SEM) observations indicated good spreading of bone marrow mesenchymal stem cells (BMSCs) in this hydrogel scaffold. Mineral nodules were found in the dog-BMSCs inoculated hydrogel by SEM after 28 days. After subcutaneous injection into nude mouse dorsum for 4 weeks, partial bone formation was observed in the chitosan/collagen/β-GP hydrogel loaded with pre-osteodifferentiated dog-BMSCs, which indicated that chitosan/collagen/β-GP hydrogel composite could induce osteodifferentiation in BMSCs without exposure to a continual supply of external osteogenic factors. In conclusion, the novel chitosan/collagen/β-GP hydrogel composite should prove useful as a bone regeneration scaffold.

Antibacterial Activity of Silver Nanoparticle-Loaded Soft Contact Lens Materials: The Effect of Monomer Composition.

PubMed

Shayani Rad, Maryam; Khameneh, Bahman; Sabeti, Zahra; Mohajeri, Seyed Ahmad; Fazly Bazzaz, Bibi Sedigheh

2016-10-01

In the present work, the effect of monomer composition on silver nanoparticles' (SNPs) binding capacity of hydrogels was investigated and their antibacterial efficacy was evaluated. Three series of poly-hydroxyethyl methacrylate (HEMA) hydrogels were prepared using methacrylic acid (MAA), methacrylamide (MAAM), and 4-vinylpyridine (4VP) as co-monomers, and ethylene glycol dimethacrylate (EGDMA) as cross-linker. SNPs binding capacity of hydrogels was evaluated in different concentrations (2, 10, and 20 ppm). In vitro antibacterial activity of SNP-loaded hydrogels was studied against Pseudomonas aeruginosa (P. aeruginosa) isolated from patients' eyes. Then, inhibitory effect of hydrogels in biofilm formation was evaluated in the presence of Staphylococcus epidermidis (S. epidermidis) (DSMZ 3270). Our data indicated that poly(HEMA-co-MAA-co-EGDMA) had superior binding affinity for SNPs in comparison with other hydrogels. All SNP-loaded hydrogels demonstrated excellent antimicrobial effects at all times against P. aeruginosa and S. epidermidis after soaking in 10 and 20 ppm SNP suspensions. Scanning electron microscope (SEM) images revealed excellent inhibitory effect of SNPs against biofilm formation on the surface of the hydrogels. This study indicated the effect of monomer compositions in SNP loading capacity of poly(HEMA) hydrogels and antibacterial efficacy of SNP-loaded hydrogels against P. aeruginosa and S. epidermidis, but further in vivo evaluation is necessary.

Mineralized polymer composites as biogenic bone substitute material

NASA Astrophysics Data System (ADS)

Shah, Rushita; Saha, Nabanita; Kitano, Takeshi; Saha, Petr

2015-05-01

Mineralized polymer composites (MPC) are recognized as potential fillers of bone defects. Though bioceramics exhibits quite a good bone-bonding and vascularization, it is considered to be too stiff and brittle for using alone. Thus, the use of polymer scaffold instead of bioceramics has several advantages including combining the osteoconductivity and bone-bonding potential of the inorganic phase with the porosity and interconnectivity of the three-dimensional construction. Aiming the advantages of ceramic-polymer composite scaffolds, the calcium carbonate (CaCO3) based biomineralized scaffold was prepared, where the PVP-CMC hydrogel was used as an extracellular matrix. This paper is reported about the morphology, swelling trend (in physiological solution) and viscoelastic behavior of (90 min mineralized) MPC. The dry MPC are off-white, coarse in texture, comparatively less flexible than the original PVP-CMC based hydrogel film, and the deposition of granular structures on the surface of the hydrogel film confirms about the development of biomineralized scaffold/polymer composites. Irrespective of thickness, the dry MPC shows higher values of swelling ratio within 30 min, which varies between 200-250 approximately. The dynamic viscoelastic nature of freshly prepared MPC was investigated applying 1% and 10% strain. At higher strain the viscoelastic moduli (G' and G") show significant change, and the nature of MPC turns from elastic to viscous. Based on the observed basic properties, the MPC (calcite based polymer composites) can be recommended for the treatment of adyanamic bone disorder.

Photocrosslinkable Gelatin/Tropoelastin Hydrogel Adhesives for Peripheral Nerve Repair.

PubMed

Soucy, Jonathan R; Shirzaei Sani, Ehsan; Portillo Lara, Roberto; Diaz, David; Dias, Felipe; Weiss, Anthony S; Koppes, Abigail N; Koppes, Ryan A; Annabi, Nasim

2018-05-09

Suturing peripheral nerve transections is the predominant therapeutic strategy for nerve repair. However, the use of sutures leads to scar tissue formation, hinders nerve regeneration, and prevents functional recovery. Fibrin-based adhesives have been widely used for nerve reconstruction, but their limited adhesive and mechanical strength and inability to promote nerve regeneration hamper their utility as a stand-alone intervention. To overcome these challenges, we engineered composite hydrogels that are neurosupportive and possess strong tissue adhesion. These composites were synthesized by photocrosslinking two naturally derived polymers, gelatin-methacryloyl (GelMA) and methacryloyl-substituted tropoelastin (MeTro). The engineered materials exhibited tunable mechanical properties by varying the GelMA/MeTro ratio. In addition, GelMA/MeTro hydrogels exhibited 15-fold higher adhesive strength to nerve tissue ex vivo compared to fibrin control. Furthermore, the composites were shown to support Schwann cell (SC) viability and proliferation, as well as neurite extension and glial cell participation in vitro, which are essential cellular components for nerve regeneration. Finally, subcutaneously implanted GelMA/MeTro hydrogels exhibited slower degradation in vivo compared with pure GelMA, indicating its potential to support the growth of slowly regenerating nerves. Thus, GelMA/MeTro composites may be used as clinically relevant biomaterials to regenerate nerves and reduce the need for microsurgical suturing during nerve reconstruction.

The Preparation and Simple Analysis of a Clay Nanoparticle Composite Hydrogel

ERIC Educational Resources Information Center

Warren, David S.; Sutherland, Sam P. H.; Kao, Jacqueline Y.; Weal, Geoffrey R.; Mackay, Sean M.

2017-01-01

Samples of a composite hydrogel incorporating clay (Laponite XLG and S-482) nanoparticles were prepared using N-isopropylacrylamide. The hydrogels were formed via a radical-initiated addition polymerization using potassium persulfate and N,N,N',N'-tetramethylethylenediamine. Students then measured the force required to stretch the gels and…

Macrosorb Kieselguhr-agarose composite adsorbents. New tools for downstream process design and scale up. Scientific note.

PubMed

Bite, M G; Berezenko, S; Reed, F J; Derry, L

1988-08-01

Incompressible Macrosorb composite adsorbents, while retaining all the desirable properties of traditional agarose-based hydrogel media, overcome the operational limitations imposed by the use of soft hydrogels: They permit useful application of fast flow rates without restrictions on bed depth and they can be used in fluidized bed mode. Considerations which are important when contemplating scaled-up processing are discussed. A comparative cost estimate for a production process for extracting albumin from bovine serum in column equipment illustrates the various advantages which may be exploited when using a composite adsorbent in place of a conventional soft gel equivalent.

Fabrication and mechanical characterization of graphene oxide-reinforced poly (acrylic acid)/gelatin composite hydrogels

NASA Astrophysics Data System (ADS)

Faghihi, Shahab; Gheysour, Mahsa; Karimi, Alireza; Salarian, Reza

2014-02-01

Hydrogels have found many practical uses in drug release, wound dressing, and tissue engineering. However, their applications are restricted due to their weak mechanical properties. The role of graphene oxide nanosheets (GONS) as reinforcement agent in poly (acrylic acid) (PAA)/Gelatin (Gel) composite hydrogels is investigated. Composite hydrogels are synthesized by thermal initiated redox polymerization method. Samples are then prepared with 20 and 40 wt. % of PAA, an increasing amount of GONS (0.1, 0.2, and 0.3 wt. %), and a constant amount of Gel. Subsequently, cylindrical hydrogel samples are subjected to a series of compression tests in order to measure their elastic modulus, maximum stress and strain. The results exhibit that the addition of GONS increases the Young's modulus and maximum stress of hydrogels significantly as compared with control (0.0 wt. % GONS). The highest Young's modulus is observed for hydrogel with GO (0.2 wt. %)/PAA (20 wt. %), whereas the highest maximum stress is detected for GO (0.2 wt. %)/PAA (40 wt. %) specimen. The addition of higher amounts of GONS leads to a decrease in the maximum stress of the hydrogel GO (0.3 wt. %)/PAA (40 wt. %). No significant differences are detected for the maximum strain among the hydrogel samples, as the amount of GONS increased. These results suggest that the application of GONS could be used to improve mechanical properties of hydrogel materials. This study may provide an alternative for the fabrication of low-cost graphene/polymer composites with enhanced mechanical properties beneficial for tissue engineering applications.

pH/NIR Light-Controlled Multidrug Release via a Mussel-Inspired Nanocomposite Hydrogel for Chemo-Photothermal Cancer Therapy

NASA Astrophysics Data System (ADS)

Ghavaminejad, Amin; Samarikhalaj, Melisa; Aguilar, Ludwig Erik; Park, Chan Hee; Kim, Cheol Sang

2016-09-01

This study reports on an intelligent composite hydrogel with both pH-dependent drug release in a cancer environment and heat generation based on NIR laser exposure, for the combined application of photothermal therapy (PTT) and multidrug chemotherapy. For the first time in the literature, Dopamine nanoparticle (DP) was incorporated as a highly effective photothermal agent as well as anticancer drug, bortezomib (BTZ) carrier inside a stimuli responsive pNIPAAm-co-pAAm hydrogel. When light is applied to the composite hydrogel, DP nanoparticle absorbs the light, which is dissipated locally as heat to impact cancer cells via hyperthermia. On the other hand, facile release of the anticancer drug BTZ from the surface of DP encapsulated hydrogel could be achieved due to the dissociation between catechol groups of DP and the boronic acid functionality of BTZ in typical acidic cancer environment. In order to increase the synergistic effect by dual drug delivery, Doxorubicin (DOXO) were also loaded to pNIPAAm-co-pAAm/DP-BTZ hydrogel and the effect of monotherapy as well as combined therapy were detailed by a complete characterization. Our results suggest that these mussel inspired nanocomposite with excellent heating property and controllable multidrug release can be considered as a potential material for cancer therapy.

Modified pineapple peel cellulose hydrogels embedded with sepia ink for effective removal of methylene blue.

PubMed

Dai, Hongjie; Huang, Huihua

2016-09-05

Novel composite hydrogels based on pineapple peel cellulose and sepia ink were synthesized by homogeneous acetylation of cellulose in ionic liquid 1-butyl-3-methylimidazolium chloride. The structure and morphology of the prepared hydrogels were characterized by Fourier transform infrared spectroscopy, field emission scanning electron microscope, X-ray diffraction, thermogravimetry and differential scanning calorimetry. The effects of acetylation time, acetylation temperature, molar ratio of acetic anhydride/anhydroglucose unit and the additive amount of sepia ink on methylene blue adsorption capacity of the hydrogels embedded with sepia ink were also investigated. Methylene blue adsorption of the hydrogels followed pseudo-second-order kinetic model and sepia ink improved adsorption capacity significantly. The adsorption capacity at equilibrium was increased from 53.72 to 138.25mg/g when the additive amount of sepia ink of the hydrogels was 10%. Copyright © 2016 Elsevier Ltd. All rights reserved.

An anisotropic hydrogel with electrostatic repulsion between cofacially aligned nanosheets

NASA Astrophysics Data System (ADS)

Liu, Mingjie; Ishida, Yasuhiro; Ebina, Yasuo; Sasaki, Takayoshi; Hikima, Takaaki; Takata, Masaki; Aida, Takuzo

2015-01-01

Machine technology frequently puts magnetic or electrostatic repulsive forces to practical use, as in maglev trains, vehicle suspensions or non-contact bearings. In contrast, materials design overwhelmingly focuses on attractive interactions, such as in the many advanced polymer-based composites, where inorganic fillers interact with a polymer matrix to improve mechanical properties. However, articular cartilage strikingly illustrates how electrostatic repulsion can be harnessed to achieve unparalleled functional efficiency: it permits virtually frictionless mechanical motion within joints, even under high compression. Here we describe a composite hydrogel with anisotropic mechanical properties dominated by electrostatic repulsion between negatively charged unilamellar titanate nanosheets embedded within it. Crucial to the behaviour of this hydrogel is the serendipitous discovery of cofacial nanosheet alignment in aqueous colloidal dispersions subjected to a strong magnetic field, which maximizes electrostatic repulsion and thereby induces a quasi-crystalline structural ordering over macroscopic length scales and with uniformly large face-to-face nanosheet separation. We fix this transiently induced structural order by transforming the dispersion into a hydrogel using light-triggered in situ vinyl polymerization. The resultant hydrogel, containing charged inorganic structures that align cofacially in a magnetic flux, deforms easily under shear forces applied parallel to the embedded nanosheets yet resists compressive forces applied orthogonally. We anticipate that the concept of embedding anisotropic repulsive electrostatics within a composite material, inspired by articular cartilage, will open up new possibilities for developing soft materials with unusual functions.

An anisotropic hydrogel with electrostatic repulsion between cofacially aligned nanosheets.

PubMed

Liu, Mingjie; Ishida, Yasuhiro; Ebina, Yasuo; Sasaki, Takayoshi; Hikima, Takaaki; Takata, Masaki; Aida, Takuzo

2015-01-01

Machine technology frequently puts magnetic or electrostatic repulsive forces to practical use, as in maglev trains, vehicle suspensions or non-contact bearings. In contrast, materials design overwhelmingly focuses on attractive interactions, such as in the many advanced polymer-based composites, where inorganic fillers interact with a polymer matrix to improve mechanical properties. However, articular cartilage strikingly illustrates how electrostatic repulsion can be harnessed to achieve unparalleled functional efficiency: it permits virtually frictionless mechanical motion within joints, even under high compression. Here we describe a composite hydrogel with anisotropic mechanical properties dominated by electrostatic repulsion between negatively charged unilamellar titanate nanosheets embedded within it. Crucial to the behaviour of this hydrogel is the serendipitous discovery of cofacial nanosheet alignment in aqueous colloidal dispersions subjected to a strong magnetic field, which maximizes electrostatic repulsion and thereby induces a quasi-crystalline structural ordering over macroscopic length scales and with uniformly large face-to-face nanosheet separation. We fix this transiently induced structural order by transforming the dispersion into a hydrogel using light-triggered in situ vinyl polymerization. The resultant hydrogel, containing charged inorganic structures that align cofacially in a magnetic flux, deforms easily under shear forces applied parallel to the embedded nanosheets yet resists compressive forces applied orthogonally. We anticipate that the concept of embedding anisotropic repulsive electrostatics within a composite material, inspired by articular cartilage, will open up new possibilities for developing soft materials with unusual functions.

Hybrid microscaffold-based 3D bioprinting of multi-cellular constructs with high compressive strength: A new biofabrication strategy

PubMed Central

Tan, Yu Jun; Tan, Xipeng; Yeong, Wai Yee; Tor, Shu Beng

2016-01-01

A hybrid 3D bioprinting approach using porous microscaffolds and extrusion-based printing method is presented. Bioink constitutes of cell-laden poly(D,L-lactic-co-glycolic acid) (PLGA) porous microspheres with thin encapsulation of agarose-collagen composite hydrogel (AC hydrogel). Highly porous microspheres enable cells to adhere and proliferate before printing. Meanwhile, AC hydrogel allows a smooth delivery of cell-laden microspheres (CLMs), with immediate gelation of construct upon printing on cold build platform. Collagen fibrils were formed in the AC hydrogel during culture at body temperature, improving the cell affinity and spreading compared to pure agarose hydrogel. Cells were proven to proliferate in the bioink and the bioprinted construct. High cell viability up to 14 days was observed. The compressive strength of the bioink is more than 100 times superior to those of pure AC hydrogel. A potential alternative in tissue engineering of tissue replacements and biological models is made possible by combining the advantages of the conventional solid scaffolds with the new 3D bioprinting technology. PMID:27966623

Highly Swellable, Dual-Responsive Hydrogels Based on PNIPAM and Redox Active Poly(ferrocenylsilane) Poly(ionic liquid)s: Synthesis, Structure, and Properties.

PubMed

Feng, Xueling; Zhang, Kaihuan; Chen, Peng; Sui, Xiaofeng; Hempenius, Mark A; Liedberg, Bo; Vancso, G Julius

2016-12-01

Highly swellable, dual-responsive hydrogels, consisting of thermo-responsive poly(N-isopropylacrylamide) (PNIPAM) and redox-responsive poly(ferrocenylsilane) (PFS) based poly(ionic liquid)s (PILs) are formed by photo-polymerization. PFS chains bearing cross-linkable vinylimidazolium (VIm) side groups are copolymerized with NIPAM in aqueous solutions under ultraviolet light (λ = 365 nm) in the presence of a photoinitiator. The PFS-PILs serve as a macro-cross-linker and also provide redox responsiveness. The swelling ratio, morphology, and lower critical solution temperature (LCST) of the hydrogels are studied as a function of the PNIPAM/PFS ratio. The value of the LCST is dependent on the choice of the counterion of the PIL and the PNIPAM/PFS ratio. The hydrogel is employed as a reducing environment for the in situ fabrication of gold nanoparticles (AuNPs), forming AuNP-hydrogel composites. The localized surface plasmon resonance peak of the as-synthesized Au nanoparticles inside the hydrogel could be tuned by altering the temperature. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Composite material

DOEpatents

Hutchens, Stacy A [Knoxville, TN; Woodward, Jonathan [Solihull, GB; Evans, Barbara R [Oak Ridge, TN; O'Neill, Hugh M [Knoxville, TN

2012-02-07

A composite biocompatible hydrogel material includes a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa. A calcium comprising salt is disposed in at least some of the pores. The porous polymer matrix can comprise cellulose, including bacterial cellulose. The composite can be used as a bone graft material. A method of tissue repair within the body of animals includes the steps of providing a composite biocompatible hydrogel material including a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa, and inserting the hydrogel material into cartilage or bone tissue of an animal, wherein the hydrogel material supports cell colonization in vitro for autologous cell seeding.

Nanoscale functionalization and characterization of surfaces with hydrogel patterns and biomolecules

NASA Astrophysics Data System (ADS)

Dinakar, Hariharasudhan Chirra

The advent of numerous tools, ease of techniques, and concepts related to nanotechnology, in combination with functionalization via simple chemistry has made gold important for various biomedical applications. In this dissertation, the development and characterization of planar gold surfaces with responsive hydrogel patterns for rapid point of care sensing and the functionalization of gold nanoparticles for drug delivery are highlighted. Biomedical micro- and nanoscale devices that are spatially functionalized with intelligent hydrogels are typically fabricated using conventional UV-lithography. Herein, precise 3-D hydrogel patterns made up of temperature responsive crosslinked poly(N-isopropylacrylamide) over gold were synthesized. The XY control of the hydrogel was achieved using microcontact printing, while thickness control was achieved using atom transfer radical polymerization (ATRP). Atomic force microscopy analysis showed that to the ATRP reaction time governed the pattern growth. The temperature dependent swelling ratio was tailored by tuning the mesh size of the hydrogel. While nanopatterns exhibited a broad lower critical solution temperature (LCST) transition, surface roughness showed a sharp LCST transition. Quartz crystal microbalance with dissipation showed rapid response behavior of the thin films, which makes them applicable as functional components in biomedical devices. The easy synthesis, relative biocompatibility, inertness, and easy functionalization of gold nanoparticles (GNPs) have made them useful for various biomedical applications. Although ATRP can be successfully carried out over GNPs, the yield of stable solution based GNPs for biomedical applications prove to be low. As an alternative approach, a novel method of ISOlating, FUnctionalizing, and REleasing nanoparticles (ISOFURE) was proposed. Biodegradable poly(beta-amino ester) hydrogels were used to synthesize ISOFURE-GNP composites. ATRP was performed inside the composite, and the final hydrogel coated GNPs were released via matrix degradation. Response analysis confirmed that the ISOFURE method led to the increased stability and yield of the hydrogel coated ISOFURE-GNPs. The ISOFURE protocol was also utilized in functionalizing GNPs with enzyme catalase in the absence of a stabilizing reagent. Biotin-streptavidin affinity was used as the bioconjugation method. Activity analysis of the conjugated enzyme showed that the ISOFURE-GNPs showed enhanced biomolecular loading relative to solution based stabilizing reagent passivated GNPs. KEYWORDS: Hydrogel, Gold nanoparticle, ISOFURE, Atom transfer radical polymerization, Microcontact printing

In situ gelable interpenetrating double network hydrogel formulated from binary components: thiolated chitosan and oxidized dextran.

PubMed

Zhang, Hanwei; Qadeer, Aisha; Chen, Weiliam

2011-05-09

In situ gelable interpenetrating double-network hydrogels composed of thiolated chitosan (Chitosan-NAC) and oxidized dextran (Odex), completely devoid of potentially cytotoxic small molecule cross-linkers and that do not require complex maneuvers or catalysis, have been formulated. The interpenetrating network structure is created by Schiff base formations and disulfide bond inter-cross-linkings through exploiting the disparity of their reaction times. Compared with the autogelable thiolated chitosan hydrogels that typically require a relatively long time span for gelation to occur, the Odex/Chitosan-NAC composition solidifies rapidly and forms a well-developed 3D network in a short time span. Compared with typical hydrogels derived from natural materials, the Odex/Chitosan-NAC hydrogels are mechanically strong and resist degradation. The cytotoxicity potential of the hydrogels was determined by an in vitro viability assay using fibroblast as a model cell, and the results reveal that the hydrogels are noncytotoxic. In parallel, in vivo results from subdermal implantation in mice models demonstrate that this hydrogel is not only highly resistant to degradation but also induces very mild tissue response.

In situ Gelable Interpenetrating Double Network Hydrogel Formulated from Binary Components: Thiolated Chitosan and Oxidized Dextran

PubMed Central

Zhang, Hanwei; Qadeer, Aisha; Chen, Weiliam

2011-01-01

In situ gelable interpenetrating double network hydrogels composed of thiolated chitosan (Chitosan-NAC) and oxidized dextran (Odex), completely devoid of potentially cytotoxic small molecule crosslinkers and do not require complex maneuvers or catalysis, have been formulated. The interpenetrating network structure is created by Schiff base formations and disulfide bond inter-crosslinkings through exploiting the disparity of their reaction times. Compare to the auto-gelable thiolated chitosan hydrogels that typically require a relatively long time span for gelation to occur, the Odex/Chitosan-NAC composition solidifies rapidly and forms a well-developed three-dimensional network in a short time span. Compare to typical hydrogels derived from natural materials, the Odex/Chitosan-NAC hydrogels are mechanically strong and resist degradation. The cytotoxicity potential of the hydrogels was determined by an in vitro viability assay using fibroblast as a model cell and the results reveal that the hydrogels are non-cytotoxic. In parallel, in vivo results from subdermal implantation in mice models demonstrate that this hydrogel is not only highly resistant to degradation but also induces very mild tissue response. PMID:21410248

Diffusion of macromolecules in self-assembled cellulose/hemicellulose hydrogels.

PubMed

Lopez-Sanchez, Patricia; Schuster, Erich; Wang, Dongjie; Gidley, Michael J; Strom, Anna

2015-05-28

Cellulose hydrogels are extensively applied in many biotechnological fields and are also used as models for plant cell walls. We synthesised model cellulosic hydrogels containing hemicelluloses, as a biomimetic of plant cell walls, in order to study the role of hemicelluloses on their mass transport properties. Microbial cellulose is able to self-assemble into composites when hemicelluloses, such as xyloglucan and arabinoxylan, are present in the incubation media, leading to hydrogels with different nano and microstructures. We investigated the diffusivities of a series of fluorescently labelled dextrans, of different molecular weight, and proteins, including a plant pectin methyl esterase (PME), using fluorescence recovery after photobleaching (FRAP). The presence of xyloglucan, known to be able to crosslink cellulose fibres, confirmed by scanning electron microscopy (SEM) and (13)C NMR, reduced mobility of macromolecules of molecular weight higher than 10 kDa, reflected in lower diffusion coefficients. Furthermore PME diffusion was reduced in composites containing xyloglucan, despite the lack of a particular binding motif in PME for this polysaccharide, suggesting possible non-specific interactions between PME and this hemicellulose. In contrast, hydrogels containing arabinoxylan coating cellulose fibres showed enhanced diffusivity of the molecules studied. The different diffusivities were related to the architectural features found in the composites as a function of polysaccharide composition. Our results show the effect of model hemicelluloses in the mass transport properties of cellulose networks in highly hydrated environments relevant to understanding the role of hemicelluloses in the permeability of plant cell walls and aiding design of plant based materials with tailored properties.

Enzymatic, urease-mediated mineralization of gellan gum hydrogel with calcium carbonate, magnesium-enriched calcium carbonate and magnesium carbonate for bone regeneration applications.

PubMed

Douglas, Timothy E L; Łapa, Agata; Samal, Sangram Keshari; Declercq, Heidi A; Schaubroeck, David; Mendes, Ana C; der Voort, Pascal Van; Dokupil, Agnieszka; Plis, Agnieszka; De Schamphelaere, Karel; Chronakis, Ioannis S; Pamuła, Elżbieta; Skirtach, Andre G

2017-12-01

Mineralization of hydrogel biomaterials is considered desirable to improve their suitability as materials for bone regeneration. Calcium carbonate (CaCO 3 ) has been successfully applied as a bone regeneration material, but hydrogel-CaCO 3 composites have received less attention. Magnesium (Mg) has been used as a component of calcium phosphate biomaterials to stimulate bone-forming cell adhesion and proliferation and bone regeneration in vivo, but its effect as a component of carbonate-based biomaterials remains uninvestigated. In the present study, gellan gum (GG) hydrogels were mineralized enzymatically with CaCO 3 , Mg-enriched CaCO 3 and magnesium carbonate to generate composite biomaterials for bone regeneration. Hydrogels loaded with the enzyme urease were mineralized by incubation in mineralization media containing urea and different ratios of calcium and magnesium ions. Increasing the magnesium concentration decreased mineral crystallinity. At low magnesium concentrations calcite was formed, while at higher concentrations magnesian calcite was formed. Hydromagnesite (Mg 5 (CO 3 ) 4 (OH) 2 .4H 2 O) formed at high magnesium concentration in the absence of calcium. The amount of mineral formed and compressive strength decreased with increasing magnesium concentration in the mineralization medium. The calcium:magnesium elemental ratio in the mineral formed was higher than in the respective mineralization media. Mineralization of hydrogels with calcite or magnesian calcite promoted adhesion and growth of osteoblast-like cells. Hydrogels mineralized with hydromagnesite displayed higher cytotoxicity. In conclusion, enzymatic mineralization of GG hydrogels with CaCO 3 in the form of calcite successfully reinforced hydrogels and promoted osteoblast-like cell adhesion and growth, but magnesium enrichment had no definitive positive effect. Copyright © 2017 John Wiley & Sons, Ltd. Copyright © 2017 John Wiley & Sons, Ltd.

Gelatin- and starch-based hydrogels. Part A: Hydrogel development, characterization and coating.

PubMed

Van Nieuwenhove, Ine; Salamon, Achim; Peters, Kirsten; Graulus, Geert-Jan; Martins, José C; Frankel, Daniel; Kersemans, Ken; De Vos, Filip; Van Vlierberghe, Sandra; Dubruel, Peter

2016-11-05

The present work aims at constructing the ideal scaffold matrix of which the physico-chemical properties can be altered according to the targeted tissue regeneration application. Ideally, this scaffold should resemble the natural extracellular matrix (ECM) as close as possible both in terms of chemical composition and mechanical properties. Therefore, hydrogel films were developed consisting of methacrylamide-modified gelatin and starch-pentenoate building blocks because the ECM can be considered as a crosslinked hydrogel network consisting of both polysaccharides and structural, signaling and cell-adhesive proteins. For the gelatin hydrogels, three different substitution degrees were evaluated including 31%, 72% and 95%. A substitution degree of 32% was applied for the starch-pentenoate building block. Pure gelatin hydrogels films as well as interpenetrating networks with gelatin and starch were developed. Subsequently, these films were characterized using gel fraction and swelling experiments, high resolution-magic angle spinning (1)H NMR spectroscopy, rheology, infrared mapping and atomic force microscopy. The results indicate that both the mechanical properties and the swelling extent of the developed hydrogel films can be controlled by varying the chemical composition and the degree of substitution of the methacrylamide-modified gelatin applied. The storage moduli of the developed materials ranged between 14 and 63kPa. Phase separation was observed for the IPNs for which separated starch domains could be distinguished located in the surrounding gelatin matrix. Furthermore, we evaluated the affinity of aggrecan for gelatin by atomic force microscopy and radiolabeling experiments. We found that aggrecan can be applied as a bioactive coating for gelatin hydrogels by a straightforward physisorption procedure. Thus, we achieved distinct fine-tuning of the physico-chemical properties of these hydrogels which render them promising candidates for tissue engineering approaches. Copyright © 2016 Elsevier Ltd. All rights reserved.

Reinforcement of mono- and bi-layer poly(ethylene glycol) hydrogels with a fibrous collagen scaffold

PubMed Central

Kinneberg, K. R. C.; Nelson, A.; Stender, M.; Aziz, A. H.; Mozdzen, L. C.; Harley, B. A. C.; Bryant, S. J.; Ferguson, V. L.

2015-01-01

Biomaterial-based tissue engineering strategies hold great promise for osteochondral tissue repair. Yet significant challenges remain in joining highly dissimilar materials to achieve a biomimetic, mechanically robust design for repairing interfaces between soft tissue and bone. This study sought to improve interfacial properties and function in a bilayer, multi-phase hydrogel interpenetrated with a fibrous collagen scaffold. ‘Soft’ 10% (w/w) and ‘stiff’ 30% (w/w) PEGDM was formed into mono- or bilayer hydrogels possessing a sharp diffusional interface. Hydrogels were evaluated as single- (hydrogel only) or multi-phase (hydrogel+fibrous scaffold penetrating throughout the stiff layer and extending >500μm into the soft layer). Including a fibrous scaffold into both soft and stiff single-phase hydrogels significantly increased tangent modulus and toughness and decreased lateral expansion under compressive loading. In multi-phase hydrogels, finite element simulations predict substantially reduced stress and strain gradients across the soft—stiff hydrogel interface. When combining two low moduli constituent material, composites theory poorly predicts the observed, large modulus increases. These results suggest material structure associated with the fibrous scaffold penetrating within the PEG hydrogel as the major contributor to improved properties and function – the hydrogel bore compressive loads and the 3D fibrous scaffold was loaded in tension thus resisting lateral expansion. PMID:26001970

In situ synthesis of bilayered gradient poly(vinyl alcohol)/hydroxyapatite composite hydrogel by directional freezing-thawing and electrophoresis method.

PubMed

Su, Cui; Su, Yunlan; Li, Zhiyong; Haq, Muhammad Abdul; Zhou, Yong; Wang, Dujin

2017-08-01

Bilayered poly(vinyl alcohol) (PVA)/hydroxyapatite (HA) composite hydrogels with anisotropic and gradient mechanical properties were prepared by the combination of directional freezing-thawing (DFT) and electrophoresis method. Firstly, PVA hydrogels with aligned channel structure were prepared by the DFT method. Then, HA nanoparticles were in situ synthesized within the PVA hydrogels via electrophoresis. By controlling the time of the electrophoresis process, a bilayered gradient hydrogel containing HA particles in only half of the gel region was obtained. The PVA/HA composite hydrogel exhibited gradient mechanical strength depending on the distance to the cathode. The gradient initial tensile modulus ranging from 0.18MPa to 0.27MPa and the gradient initial compressive modulus from 0.33MPa to 0.51MPa were achieved. The binding strength of the two regions was relatively high and no apparent internal stress or defect was observed at the boundary. The two regions of the bilayered hydrogel also showed different osteoblast cell adhesion properties. Copyright © 2017 Elsevier B.V. All rights reserved.

Cellularized cylindrical fiber/hydrogel composites for ligament tissue engineering.

PubMed

Thayer, Patrick S; Dimling, Anna F; Plessl, Daniel S; Hahn, Mariah R; Guelcher, Scott A; Dahlgren, Linda A; Goldstein, Aaron S

2014-01-13

Electrospun meshes suffer from poor cell infiltration and limited thickness, which restrict their use to thin tissue applications. Herein, we demonstrate two complementary processes to overcome these limitations and achieve elastomeric composites that may be suitable for ligament repair. First, C3H10T1/2 mesenchymal stem cells were incorporated into electrospun meshes using a hybrid electrospinning/electrospraying process. Second, electrospun meshes were rolled and formed into composites with an interpenetrating polyethylene glycol (PEG) hydrogel network. Stiffer composites were formed from poly(lactic-co-glycolic acid) (PLGA) meshes, while softer and more elastic composites were formed from poly(ester-urethane urea) (PEUUR) meshes. As-spun PLGA and PEUUR rolled meshes had tensile moduli of 19.2 ± 1.9 and 0.86 ± 0.34 MPa, respectively, which changed to 11.6 ± 4.8 and 1.05 ± 0.39 MPa with the incorporation of a PEG hydrogel phase. In addition, cyclic tensile testing indicated that PEUUR-based composites deformed elastically to at least 10%. Finally, C3H10T1/2 cells incorporated into electrospun meshes survived the addition of the PEG phase and remained viable for up to 5 days. These results indicate that the fabricated cellularized composites are support cyclic mechanical conditioning, and have potential application in ligament repair.

A bioprintable form of chitosan hydrogel for bone tissue engineering.

PubMed

Demirtaş, Tuğrul Tolga; Irmak, Gülseren; Gümüşderelioğlu, Menemşe

2017-07-13

Bioprinting can be defined as 3D patterning of living cells and other biologics by filling and assembling them using a computer-aided layer-by-layer deposition approach to fabricate living tissue and organ analogs for tissue engineering. The presence of cells within the ink to use a 'bio-ink' presents the potential to print 3D structures that can be implanted or printed into damaged/diseased bone tissue to promote highly controlled cell-based regeneration and remineralization of bone. In this study, it was shown for the first time that chitosan solution and its composite with nanostructured bone-like hydroxyapatite (HA) can be mixed with cells and printed successfully. MC3T3-E1 pre-osteoblast cell laden chitosan and chitosan-HA hydrogels, which were printed with the use of an extruder-based bioprinter, were characterized by comparing these hydrogels to alginate and alginate-HA hydrogels. Rheological analysis showed that all groups had viscoelastic properties. It was also shown that under simulated physiological conditions, chitosan and chitosan-HA hydrogels were stable. Also, the viscosity values of the bio-solutions were in an applicable range to be used in 3D bio-printers. Cell viability and proliferation analyses documented that after printing with bio-solutions, cells continued to be viable in all groups. It was observed that cells printed within chitosan-HA composite hydrogel had peak expression levels for early and late stages osteogenic markers. It was concluded that cells within chitosan and chitosan-HA hydrogels had mineralized and differentiated osteogenically after 21 days of culture. It was also discovered that chitosan is superior to alginate, which is the most widely used solution preferred in bioprinting systems, in terms of cell proliferation and differentiation. Thus, applicability and printability of chitosan as a bio-printing solution were clearly demonstrated. Furthermore, it was proven that the presence of bone-like nanostructured HA in alginate and chitosan hydrogels improved cell viability, proliferation and osteogenic differentiation.

Investigation of Magnetic Properties and Mechanical Responses on Hydrogel-TMAH-Magnetite

NASA Astrophysics Data System (ADS)

Sunaryono; Hidayat, M. F.; Insjaf, C.; Taufiq, A.; Mufti, N.; Munasir

2018-05-01

Hydrogel-TMAH-Magnetite (ferrogel) was fabricated by using polyvinyl alcohol (PVA) hydrogel and magnetite fluids with tetramethylammonium hydroxide (TMAH) surfactant. Iron sand as the raw material was used to synthesize magnetite nanoparticles by co-precipitation method. Magnetite nanoparticles and ferrogel were characterized using X-Ray Fluorescence (XRF) to determine the content of elements in it. To know the functional group network of magnetite nanoparticles, magnetite enclosed with TMAH and ferrogel; we investigated using Fourier Transform Infra-Red (FTIR). Meanwhile, the magnetic properties of the hydrogel-TMAH-magnetite were measured by using Vibrating Sample Magnetometer (VSM). Furthermore, the composition analysis of the ferrogels using FTIR showed that all the synthesis materials were inside the ferrogels. The saturation magnetization of the hydrogel-TMAH-magnetite with a composition of TMAH 1.2 mL (3.95 emu·g-1) was higher than that of TMAH 0.8 mL (0.85 emu·g-1). It exhibited that the composition of TMAH 1.2 mL was an optimum composition to produce nanoparticle magnetite-TMAH having a stable and high performance. Furthermore, the magneto-elasticity of hydrogel-TMAH-magnetite in the effect of the external magnetic field had a good response. However, the composition of the nanoparticle magnetite-TMAH in the ferrogel did not significantly affect the elongation of the gel.

The composite hydrogels of polyvinyl alcohol-gellan gum-Ca(2+) with improved network structure and mechanical property.

PubMed

Wang, Fei; Wen, Ying; Bai, Tongchun

2016-12-01

The composite hydrogels of polyvinyl alcohol (PVA) and gellan gum (GG) are of interesting in the biomaterials application. To improve the structure and mechanical property, in this work, Ca(2+) ion was introduced to crosslink the polymer chain, and the PVA-GG-Ca(2+) hydrogel was formed. By analyzing its structure, mechanical properties, swelling and dehydration kinetics, the effect of molecular interaction on hydrogel structure and properties have been observed. Our result indicates that, as GG is added to hydrogel network, the role of Ca(2+) ion is stand out, it reorganizes the network structure, enhances the mechanical properties, and strengthens the electrolytic and hydrogen bonding interactions in PVA-GG-Ca(2+) hydrogels. These observations will benefit the development of hydrogels in biomaterials application. Copyright © 2016. Published by Elsevier B.V.

Temperature responsive hydrogel magnetic nanocomposites for hyperthermia and metal extraction applications

NASA Astrophysics Data System (ADS)

Reddy, N. Narayana; Ravindra, S.; Reddy, N. Madhava; Rajinikanth, V.; Raju, K. Mohana; Vallabhapurapu, Vijaya Srinivasu

2015-11-01

The present work deals with the development of temperature and magnetic responsive hydrogel networks based on poly (N-isopropylacrylamide)/acrylamido propane sulfonic acid. The hydrogel matrices are synthesized by polymerizing N-isopropylacrylamide (NIPAM) monomer in the presence of acrylamido propane sulphonicacid (AMPS) using a cross-linker (N,N-methylenebisacrylamide, MBA) and redox initiating system [ammonium persulphate (APS)/tetramethylethylenediamine (TMEDA)]. The magnetic nanoparticles are generated throughout the hydrogel networks using in situ method by incorporating iron ions and subsequent treatment with ammonia. A series of hydrogel-magnetic nanocomposites (HGMNC) are developed by varying AMPS composition. The synthesized hydrogel magnetic nanocomposites (HGMNC) are characterized by using Fourier Transform Infrared (FTIR) Spectroscopy, X-ray diffraction (XRD), Thermal Analyses and Electron Microscopy analysis (Scanning and Transmission Electron Microscope). The metal extraction capacities of the prepared hydrogel (HG) and hydrogel magnetic nanocomposites (HGMNC) were studied at different temperatures. The results suggest that HGMNCs have higher extraction capacity compared to HG and HG loaded iron ions. This data also reveals that the extraction of metals by hydrogel magnetic nanocomposites (HGMNCs) is higher at higher temperatures than room temperature. The prepared HGMNCs are also subjected to hyperthermia (cancer therapy) studies.

Novel injectable gellan gum hydrogel composites incorporating Zn- and Sr-enriched bioactive glass microparticles: High-resolution X-ray microcomputed tomography, antibacterial and in vitro testing.

PubMed

Douglas, Timothy E L; Dziadek, Michal; Gorodzha, Svetlana; Lišková, Jana; Brackman, Gilles; Vanhoorne, Valérie; Vervaet, Chris; Balcaen, Lieve; Del Rosario Florez Garcia, Maria; Boccaccini, Aldo R; Weinhardt, Venera; Baumbach, Tilo; Vanhaecke, Frank; Coenye, Tom; Bačáková, Lucie; Surmeneva, Maria A; Surmenev, Roman A; Cholewa-Kowalska, Katarzyna; Skirtach, Andre G

2018-06-01

Mineralization of hydrogel biomaterials is desirable to improve their suitability as materials for bone regeneration. In this study, gellan gum (GG) hydrogels were formed by simple mixing of GG solution with bioactive glass microparticles of 45S5 composition, leading to hydrogel formation by ion release from the amorphous bioactive glass microparticles. This resulted in novel injectable, self-gelling composites of GG hydrogels containing 20% bioactive glass. Gelation occurred within 20 min. Composites containing the standard 45S5 bioactive glass preparation were markedly less stiff. X-ray microcomputed tomography proved to be a highly sensitive technique capable of detecting microparticles of diameter approximately 8 μm, that is, individual microparticles, and accurately visualizing the size distribution of bioactive glass microparticles and their aggregates, and their distribution in GG hydrogels. The widely used melt-derived 45S5 preparation served as a standard and was compared with a calcium-rich, sol-gel derived preparation (A2), as well as A2 enriched with zinc (A2Zn5) and strontium (A2Sr5). A2, A2Zn, and A2Sr bioactive glass particles were more homogeneously dispersed in GG hydrogels than 45S5. Composites containing all four bioactive glass preparations exhibited antibacterial activity against methicillin-resistant Staphylococcus aureus. Composites containing A2Zn5 and A2Sr5 bioactive glasses supported the adhesion and growth of osteoblast-like cells and were considerably more cytocompatible than 45S5. All composites underwent mineralization with calcium-deficient hydroxyapatite upon incubation in simulated body fluid. The extent of mineralization appeared to be greatest for composites containing A2Zn5 and 45S5. The results underline the importance of the choice of bioactive glass when preparing injectable, self-gelling composites. Copyright © 2018 John Wiley & Sons, Ltd.

Method of tissue repair using a composite material

DOEpatents

Hutchens, Stacy A.; Woodward, Jonathan; Evans, Barbara R.; O'Neill, Hugh M.

2016-03-01

A composite biocompatible hydrogel material includes a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa. A calcium comprising salt is disposed in at least some of the pores. The porous polymer matrix can comprise cellulose, including bacterial cellulose. The composite can be used as a bone graft material. A method of tissue repair within the body of animals includes the steps of providing a composite biocompatible hydrogel material including a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa, and inserting the hydrogel material into cartilage or bone tissue of an animal, wherein the hydrogel material supports cell colonization in vitro for autologous cell seeding.

Method of tissue repair using a composite material

DOEpatents

Hutchens, Stacy A; Woodward, Jonathan; Evans, Barbara R; O'Neill, Hugh M

2014-03-18

A composite biocompatible hydrogel material includes a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa. A calcium comprising salt is disposed in at least some of the pores. The porous polymer matrix can comprise cellulose, including bacterial cellulose. The composite can be used as a bone graft material. A method of tissue repair within the body of animals includes the steps of providing a composite biocompatible hydrogel material including a porous polymer matrix, the polymer matrix including a plurality of pores and providing a Young's modulus of at least 10 GPa, and inserting the hydrogel material into cartilage or bone tissue of an animal, wherein the hydrogel material supports cell colonization in vitro for autologous cell seeding.

Rapid shape memory TEMPO-oxidized cellulose nanofibers/polyacrylamide/gelatin hydrogels with enhanced mechanical strength.

PubMed

Li, Nan; Chen, Wei; Chen, Guangxue; Tian, Junfei

2017-09-01

TEMPO-oxidized cellulose nanofibers/polyacrylamide/gelatin shape memory hydrogels were successfully fabricated through a facile in-situ free-radical polymerization method, and double network was formed by chemically cross-linked polyacrylamide (PAM) network and physically cross-linked gelatin network. TEMPO-oxidized cellulose nanofibers (TOCNs) were introduced to improve the mechanical properties of the hydrogel. The structure, shape memory behaviors and mechanical properties of the resulting composite gels with varied gel compositions were investigated. The results obtained from those different studies revealed that TOCNs, gelatin, and PAM could mix with each other homogeneously. Due to the thermoreversible nature of the gelatin network, the composite hydrogels exhibited attractive thermo-induced shape memory properties. In addition, good mechanical properties (strength >200kPa, strain >650%) were achieved. Such composite hydrogels with good shape memory behavior and enhanced mechanical strength would be an attractive candidate for a wide variety of applications. Copyright © 2017 Elsevier Ltd. All rights reserved.

Biodegradable synthetic bone composites

DOEpatents

Liu, Gao; Zhao, Dacheng; Saiz, Eduardo; Tomsia, Antoni P.

2013-01-01

The invention provides for a biodegradable synthetic bone composition comprising a biodegradable hydrogel polymer scaffold comprising a plurality of hydrolytically unstable linkages, and an inorganic component; such as a biodegradable poly(hydroxyethylmethacrylate)/hydroxyapatite (pHEMA/HA) hydrogel composite possessing mineral content approximately that of human bone.

On the Interaction between Superabsorbent Hydrogels and Cementitious Materials

NASA Astrophysics Data System (ADS)

Farzanian, Khashayar

Autogenous shrinkage induced cracking is a major concern in high performance concretes (HPC), which are produced with low water to cement ratios. Internal curing to maintain high relative humidity in HPC with the use of an internal water reservoir has proven effective in mitigating autogenous shrinkage in HPC. Superabsorbent polymers (SAP) or hydrogels have received increasing attention as an internal curing agent in recent years. A key advantage of SAP is its versatility in size distribution and absorption/desorption characteristics, which allow it to be adapted to specific mix designs. Understanding the behavior of superabsorbent hydrogels in cementitious materials is critical for accurate design of internal curing. The primary goal of this study is to fundamentally understand the interaction between superabsorbent hydrogels and cementitious materials. In the first step, the effect of chemical and mechanical conditions on the absorption of hydrogels is investigated. In the second step, the desorption of hydrogels in contact with porous cementitious materials is examined to aid in understanding the mechanisms of water release from superabsorbent hydrogels (SAP) into cementitious materials. The dependence of hydrogel desorption on the microstructure of cementitious materials and relative humidity is studied. It is shown that the capillary forces developed at the interface between the hydrogel and cementitious materials increased the desorption of the hydrogels. The size of hydrogels is shown to influence desorption, beyond the known size dependence of bulk diffusion, through debonding from the cementitious matrix, thereby decreasing the effect of the Laplace pressure on desorption. In the third step, the desorption of hydrogels synthesized with varied chemical compositions in cementitious materials are investigated. The absorption, chemical structure and mechanical response of hydrogels swollen in a cement mixture are studied. The effect of the capillary forces on the desorption of hydrogels is investigated in relation to the chemical composition of the hydrogels. In the second set of experiments of this part, the behavior of the hydrogels in a hydrating cement paste is monitored by tracking the size and morphology evolution of hydrogels interacting with the cement paste matrix. It is shown that the changes on the surface characteristics of hydrogels as a result of interactions with the pore solution and cement particles can affect the desorption rate of hydrogels in contact with a porous cementitious material. Scanning electron microscopic (SEM) examination demonstrates two different desorption modes with distinct morphologies of hydrogels depending on the chemical composition of hydrogels. The effect of the interfacial bonding between the hydrogels and the cementitious matrix and its relation to the desorption is illustrated. The desorption of hydrogels with different chemical compositions in blended cement mixture containing different supplementary cementitious materials (SCMs) such as slag, fly ash, silica fume and two types of glass powders, are examined. The absorption/desorption kinetics of hydrogels in different hydrating blended cement mixtures are monitored by freeze drying the samples at different times. The surface characteristics of different hydrogels after interaction with pore solution, cement particles and SCMs particles are examined and their relation to interfacial bonding is illustrated. It is shown that different SCMs can cause distinct changes on interfacial bonding. The understanding of hydrogel behavior in cementitious materials helps with accurate mixture design for internal curing. The kinetics of desorption is crucial for the purpose of internal curing. The understanding of release mechanisms and the change in the hydrogel morphology is important for the self-healing and self-sealing applications. Two major contributions of this research are (1) to show the effect of capillary forces developed at the interface between cementitious matrix and hydrogel which can increase the rate of desorption dramatically and (2) to illustrate the chemo-physical interaction between cement pore solution and hydrating particles with hydrogels which can affect the interfacial bonding between hydrogel and cement. These two main contributions will be useful to understand the absorption and desorption behavior of hydrogel in cementitious materials. Two main strengths of experimental procedures of this research are (1) use of in-house synthesis of hydrogels that permits establishing a link between the chemical composition of hydrogels and their behavior in cementitious materials and (2) use of freeze drying for the first time to monitor the behavior of hydrogels interacting with a hydrating cementitious matrix.

Three-dimensional printing fiber reinforced hydrogel composites.

PubMed

Bakarich, Shannon E; Gorkin, Robert; in het Panhuis, Marc; Spinks, Geoffrey M

2014-09-24

An additive manufacturing process that combines digital modeling and 3D printing was used to prepare fiber reinforced hydrogels in a single-step process. The composite materials were fabricated by selectively pattering a combination of alginate/acrylamide gel precursor solution and an epoxy based UV-curable adhesive (Emax 904 Gel-SC) with an extrusion printer. UV irradiation was used to cure the two inks into a single composite material. Spatial control of fiber distribution within the digital models allowed for the fabrication of a series of materials with a spectrum of swelling behavior and mechanical properties with physical characteristics ranging from soft and wet to hard and dry. A comparison with the "rule of mixtures" was used to show that the swollen composite materials adhere to standard composite theory. A prototype meniscus cartilage was prepared to illustrate the potential application in bioengineering.

Smart hydrogel-functionalized textile system with moisture management property for skin application

NASA Astrophysics Data System (ADS)

Wang, Xiaowen; Hu, Huawen; Yang, Zongyue; He, Liang; Kong, Yeeyee; Fei, Bin; Xin, John H.

2014-12-01

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 (ɛ-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.

Formulation of sage essential oil (Salvia officinalis, L.) monoterpenes into chitosan hydrogels and permeation study with GC-MS analysis.

PubMed

Kodadová, Alexandra; Vitková, Zuzana; Herdová, Petra; Ťažký, Anton; Oremusová, Jarmila; Grančai, Daniel; Mikuš, Peter

2015-01-01

This study deals with the formulation of natural drugs into hydrogels. For the first time, compounds from the sage essential oil were formulated into chitosan hydrogels. A sample preparation procedure for hydrophobic volatile analytes present in a hydrophilic water matrix along with an analytical method based on the gas chromatography coupled with the mass spectrometry (GC-MS) was developed and applied for the evaluation of the identity and quantity of essential oil components in the hydrogels and saline samples. The experimental results revealed that the chitosan hydrogels are suitable for the formulation of sage essential oil. The monoterpene release can be effectively controlled by both chitosan and caffeine concentration in the hydrogels. Permeation experiment, based on a hydrogel with the optimized composition [3.5% (w/w) sage essential oil, 2.0% (w/w) caffeine, 2.5% (w/w) chitosan and 0.1% (w/w) Tween-80] in donor compartment, saline solution in acceptor compartment, and semi-permeable cellophane membrane, demonstrated the useful permeation selectivity. Here, (according to lipophilicity) an enhanced permeation of the bicyclic monoterpenes with antiflogistic and antiseptic properties (eucalyptol, camphor and borneol) and, at the same time, suppressed permeation of toxic thujone (not exceeding its permitted applicable concentration) was observed. These properties highlight the pharmaceutical importance of the developed chitosan hydrogel formulating sage essential oil in the dermal applications.

Development of hydrogels for regenerative engineering.

PubMed

Guan, Xiaofei; Avci-Adali, Meltem; Alarçin, Emine; Cheng, Hao; Kashaf, Sara Saheb; Li, Yuxiao; Chawla, Aditya; Jang, Hae Lin; Khademhosseini, Ali

2017-05-01

The aim of regenerative engineering is to restore complex tissues and biological systems through convergence in the fields of advanced biomaterials, stem cell science, and developmental biology. Hydrogels are one of the most attractive biomaterials for regenerative engineering, since they can be engineered into tissue mimetic 3D scaffolds to support cell growth due to their similarity to native extracellular matrix. Advanced nano- and micro-technologies have dramatically increased the ability to control properties and functionalities of hydrogel materials by facilitating biomimetic fabrication of more sophisticated compositions and architectures, thus extending our understanding of cell-matrix interactions at the nanoscale. With this perspective, this review discusses the most commonly used hydrogel materials and their fabrication strategies for regenerative engineering. We highlight the physical, chemical, and functional modulation of hydrogels to design and engineer biomimetic tissues based on recent achievements in nano- and micro-technologies. In addition, current hydrogel-based regenerative engineering strategies for treating multiple tissues, such as musculoskeletal, nervous and cardiac tissue, are also covered in this review. The interaction of multiple disciplines including materials science, cell biology, and chemistry, will further play an important role in the design of functional hydrogels for the regeneration of complex tissues. Copyright © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

New composite thixotropic hydrogel composed of a polymer hydrogelator and a nanosheet

NASA Astrophysics Data System (ADS)

Ohsedo, Yutaka; Oono, Masashi; Saruhashi, Kowichiro; Watanabe, Hisayuki; Miyamoto, Nobuyoshi

2017-12-01

A composite gel composed of a water-soluble aromatic polyamide hydrogelator and the nanosheet Laponite®, a synthetic layered silicate, was produced and found to exhibit thixotropic behaviour. Whereas the composite gel contains the gelator at the same concentration as the molecular gel made by the gelator only, the composite gel becomes a softer thixotropic gel compared to the molecular gel made by the gelator only. The reason for this could be that bundles of polymer gelator may be loosened and the density of the polymer network increased in the presence of Laponite.

New composite thixotropic hydrogel composed of a polymer hydrogelator and a nanosheet

PubMed Central

Oono, Masashi; Saruhashi, Kowichiro; Watanabe, Hisayuki; Miyamoto, Nobuyoshi

2017-01-01

A composite gel composed of a water-soluble aromatic polyamide hydrogelator and the nanosheet Laponite®, a synthetic layered silicate, was produced and found to exhibit thixotropic behaviour. Whereas the composite gel contains the gelator at the same concentration as the molecular gel made by the gelator only, the composite gel becomes a softer thixotropic gel compared to the molecular gel made by the gelator only. The reason for this could be that bundles of polymer gelator may be loosened and the density of the polymer network increased in the presence of Laponite. PMID:29308249

Effects of konjac glucomannan on the structure, properties, and drug release characteristics of agarose hydrogels.

PubMed

Yuan, Yi; Wang, Lin; Mu, Ruo-Jun; Gong, Jingni; Wang, Yuyan; Li, Yuanzhao; Ma, Jiaqi; Pang, Jie; Wu, Chunhua

2018-06-15

Pure agarose (AG) hydrogels have strong rigidity and brittleness, which greatly limit their applications. Therefore, in this study, konjac glucomannan (KGM) was used to improve the properties of AG hydrogels. The effect of KGM on the structure and properties of AG hydrogels was investigated by rotational rheometry, Fourier Transform Infrared Spectroscopy, X-ray Diffraction, and Scanning Electron Microscopy. The results showed that the flexibility of the composite hydrogels increases with KGM concentration, which may be attributed to a synergistic interaction between KGM and AG resulting in a compact network structure. In vitro drug release behavior of composite hydrogels was investigated under different environments using model drug ciprofloxacin. The results showed that the encapsulation, drug loading efficiencies, and sustained release capacity of AG hydrogels were enhanced by the incorporation of KGM. These results suggested that KGM has the potential to enhance the properties and drug release characteristics of AG hydrogels. Copyright © 2018 Elsevier Ltd. All rights reserved.

Shape morphing and motion of responsive hydrogel composites

NASA Astrophysics Data System (ADS)

Hayward, Ryan

Composites of stimuli-responsive hydrogels paired with stiff structural elements or functional inorganic materials offer myriad opportunities to control the shape, properties, and motion of materials. In one example, our group has studied the geometry and mechanics of swelling-induced buckling of polymer trilayer films consisting of patterning rigid layers sandwiching a swellable hydrogel layer. Of particular recent interest has been the formation of helical structures from seedpod-type architectures with perpendicular orientation of stripes on opposite faces. We have studied the concatenation of two or more helical segments, yielding simple geometric design rules for the fabrication of 3D constructs. In a second example, we have considered the light-driven reshaping and motion of hydrogels containing plasmonic nanoparticles as photothermal heating elements. In contrast to systems pre-programmed to take on a single, or perhaps a few, different 3D shapes, this approach enables continuous shape reconfiguration, and correspondingly, directed motion of composite hydrogel sheets.

Biomimetic membrane arrays on cast hydrogel supports.

PubMed

Roerdink Lander, Monique; Ibragimova, Sania; Rein, Christian; Vogel, Jörg; Stibius, Karin; Geschke, Oliver; Perry, Mark; Hélix-Nielsen, Claus

2011-06-07

Lipid bilayers are intrinsically fragile and require mechanical support in technical applications based on biomimetic membranes. Tethering the lipid bilayer membranes to solid substrates, either directly through covalent or ionic substrate-lipid links or indirectly on substrate-supported cushions, provides mechanical support but at the cost of small molecule transport through the membrane-support sandwich. To stabilize biomimetic membranes while allowing transport through a membrane-support sandwich, we have investigated the feasibility of using an ethylene tetrafluoroethylene (ETFE)/hydrogel sandwich as the support. The sandwich is realized as a perforated surface-treated ETFE film onto which a hydrogel composite support structure is cast. We report a simple method to prepare arrays of lipid bilayer membranes with low intrinsic electrical conductance on the highly permeable, self-supporting ETFE/hydrogel sandwiches. We demonstrate how the ETFE/hydrogel sandwich support promotes rapid self-thinning of lipid bilayers suitable for hosting membrane-spanning proteins.

Wood mimetic hydrogel beads for enzyme immobilization.

PubMed

Park, Saerom; Kim, Sung Hee; Won, Keehoon; Choi, Joon Weon; Kim, Yong Hwan; Kim, Hyung Joo; Yang, Yung-Hun; Lee, Sang Hyun

2015-01-22

Wood component-based composite hydrogels have potential applications in biomedical fields owing to their low cost, biodegradability, and biocompatibility. The controllable properties of wood mimetic composites containing three major wood components are useful for enzyme immobilization. Here, lipase from Candida rugosa was entrapped in wood mimetic beads containing cellulose, xylan, and lignin by dissolving wood components with lipase in [Emim][Ac], followed by reconstitution. Lipase entrapped in cellulose/xylan/lignin beads in a 5:3:2 ratio showed the highest activity; this ratio is very similar to that in natural wood. The lipase entrapped in various wood mimetic beads showed increased thermal and pH stability. The half-life times of lipase entrapped in cellulose/alkali lignin hydrogel were 31- and 82-times higher than those of free lipase during incubation under denaturing conditions of high temperature and low pH, respectively. Owing to their biocompatibility, biodegradability, and controllable properties, wood mimetic hydrogel beads can be used to immobilize various enzymes for applications in the biomedical, bioelectronic, and biocatalytic fields. Copyright © 2014 Elsevier Ltd. All rights reserved.

A cotton fabric modified with a hydrogel containing ZnO nanoparticles. Preparation and properties study

NASA Astrophysics Data System (ADS)

Staneva, Desislava; Atanasova, Daniela; Vasileva-Tonkova, Evgenia; Lukanova, Varbina; Grabchev, Ivo

2015-08-01

Two different methods were used to obtain composite materials based on a ZnO nanoparticles-hydrogel-cotton fabric. The hydrogels, synthesized by photopolymerization, were utilized to provide uniform distribution and binding of the nanoparticles to the fiber surface and to prevent their agglomeration. N-methyldiethanolamine (MDEA) was used as a co-initiator in hydrogel photopolymerization and as an alkaline agent in the synthesis of ZnO nanoparticles. Due to the difference in size, shape and morphology of the nanoparticles, examined by a TEM and SEM, it was found that the materials have distinct photoluminescence properties, e.g. in the entire visible or UV range. The composite materials with small size nanoparticles and photoluminescence in near UV range were investigated for antibiotic activity against the bacterial strains Pseudomonas aeruginosa and Acinetobacter johnsonii known as important pathogens in clinical infections. Significantly high antibacterial effect on the bacteria tested was achieved, especially on A. johnsonii. This suggests potential application of the new formulations as effective wound dressings to control the spread of infections.

Synthesis of polymer ion-exchange hydrogels under γ - irradiation 60Co

NASA Astrophysics Data System (ADS)

Le, V. M.; Zhevnyak, V. D.; Pak, V. Kh; Ananev, V. A.; Borodin, U. V.

2015-04-01

We have reported earlier about the modification of ion-exchange hydrogel under the influence of gamma radiation. The optimal absorbed dose of irradiation had been choosen for radiation modification of polymer hydrogels by ionits to produce products with a high content of the gel - fractions and sufficient mechanical properties. The dependence of the static exchange capacity of hydrogels on the type of ionit and its fractional composition had been studied. The dependence of the static exchange capacity of the quantitative composition of the ionit in the volume of the hydrogel had been investigated. The ion-exchange medical eye lenses had been made under selected conditions of synthesis. Their sorption properties had been studied.

ADVANCED MOLECULAR DESIGN OF BIOPOLYMERS FOR TRANSMUCOSAL AND INTRACELLULAR DELIVERY OF CHEMOTHERAPEUTIC AGENTS AND BIOLOGICAL THERAPEUTICS

PubMed Central

Liechty, William B.; Caldorera-Moore, Mary; Phillips, Margaret A.; Schoener, Cody; Peppas, Nicholas A.

2011-01-01

Hydrogels have been instrumental in the development of polymeric systems for controlled release of therapeutic agents. These materials are attractive for transmucosal and intracellular drug delivery because of their facile synthesis, inherent biocompatibility, tunable physicochemical properties, and capacity to respond to various physiological stimuli. In this contribution, we outline a multifaceted hydrogel-based approach for expanding the range of therapeutics in oral formulations from classical small-molecule drugs to include proteins, chemotherapeutics, and nucleic acids. Through judicious materials selection and careful design of copolymer composition and molecular architecture, we can engineer systems capable of responding to distinct physiological cues, with tunable physicochemical properties that are optimized to load, protect, and deliver valuable macromolecular payloads to their intended site of action. These hydrogel carriers, including complexation hydrogels, tethered hydrogels, interpenetrating networks, nanoscale hydrogels, and hydrogels with decorated structures are investigated for their ability respond to changes in pH, to load and release insulin and fluorescein, and remain non-toxic to Caco-2 cells. Our results suggest these novel hydrogel networks have great potential for controlled delivery of proteins, chemotherapeutics, and nucleic acids. PMID:21699934

Temperature-responsive in situ nanoparticle hydrogels based on hydrophilic pendant cyclic ether modified PEG-PCL-PEG.

PubMed

Feng, Zujian; Zhao, Junqiang; Li, Yin; Xu, Shuxin; Zhou, Junhui; Zhang, Jianhua; Deng, Liandong; Dong, Anjie

2016-10-20

Thermo-sensitive injectable hydrogels based on poly(ε-caprolactone)/poly(ethylene glycol) (PCL/PEG) block copolymers have attracted considerable attention for sustained drug release and tissue engineering applications. Previously, we have reported a thermo-sensitive hydrogel of P(CL-co-TOSUO)-PEG-P(CL-co-TOSUO) (PECT) triblock copolymers modified by hydrophilic cyclic ether pendant groups 1,4,8-trioxa-[4.6]spiro-9-undecanone (TOSUO). Unfortunately, the low gel modulus of PECT (only 50-70 Pa) may limit its applications. Herein, another kind of thermogelling triblock copolymer of a pendant cyclic ether-modified caprolactonic poloxamer analog, PEG-P(CL-co-TOSUO)-PEG (PECTE), was successfully prepared by control of the hydrophilicity/hydrophobicity balance and chemical compositions of the copolymers. PECTE powder could directly disperse in water to form a stable nanoparticle (NP) aqueous dispersion and underwent sol-gel-sol transition behavior at a higher concentration with the temperature increasing from ambient or lower temperatures. Significantly, the microstructure parameters (e.g., different chemical compositions of the hydrophobic block and topology) played a critical role in the phase transition behavior. Furthermore, comparison studies on PECTE and PEG-PCL-PEG (PECE) showed that the introduction of pendant cyclic ether groups into PCL blocks could avoid unexpected ahead-of-time gelling of the PECE aqueous solution. In addition, the rheological analysis of PECTE and PECT indicated that the storage modulus of the PECTE hydrogel could be 100 times greater than that of the PECT hydrogel under the same mole ratios of TOSUO/CL and lower molecular weight. Consequently, PECTE thermal hydrogel systems are believed to be promising as in situ gel-forming biomaterials for drug delivery and tissue engineering.

Study of the effect of mixing approach on cross-linking efficiency of hyaluronic acid-based hydrogel cross-linked with 1,4-butanediol diglycidyl ether.

PubMed

Al-Sibani, Mohammed; Al-Harrasi, Ahmed; Neubert, Reinhard H H

2016-08-25

Regardless of various strategies reported for cross-linking hyaluronic acid (HA) with 1,4-butanediol diglycidyl ether (BDDE), seeking new strategies that enhance cross-linking efficiency with a low level of cross-linker is essential. In this work, we studied the influence of mixing approach on two cross-linked BDDE-HA hydrogels prepared by two different mixing approaches; the large-batch mixing approach in which the hydrogel quantities were all mixed as a single lump in one container (hydrogel 1), and the small-batches mixing approach in which the hydrogel quantities were divided into smaller batches, mixed separately at various HA/BDDE ratios then combined in one reaction mixture (hydrogel 2). The result showed that the cross-linking reaction was mixing process-dependent. Degradation tests proved that, in relation to hydrogel 1, hydrogel 2 was more stable, and exhibited a higher resistance towards hyaluronidase activity. The swelling ratio of hydrogel 1 was significantly higher than that of hydrogel 2 in distilled water; however, in phosphate buffer saline, both hydrogels showed no significant difference. SEM images demonstrated that hydrogel 2 composite showed a denser network structure and smaller pore-size than hydrogel 1. In comparison to native HA, the occurrence of chemical modification in the cross-linked hydrogels was confirmed by FTIR and NMR distinctive peaks. These peaks also provided evidence that hydrogel 2 exhibited a higher degree of modification than hydrogel 1. In conclusion, the small-batches mixing approach proved to be more effective than large-batch mixing in promoting HA-HA entanglement and increasing the probability of BDDE molecules for binding with HA chains. Copyright © 2016 Elsevier B.V. All rights reserved.

Composite hydrogel of chitosan-poly(hydroxybutyrate-co-valerate) with chondroitin sulfate nanoparticles for nucleus pulposus tissue engineering.

PubMed

Nair, Manitha B; Baranwal, Gaurav; Vijayan, Prajuna; Keyan, Kripa S; Jayakumar, R

2015-12-01

Intervertebral disc degeneration, occurring mainly in nucleus pulposus (NP), is a leading cause of low back pain. In seeking to mitigate this condition, investigators in the field of NP tissue engineering have increasingly studied the use of hydrogels. However, these hydrogels should possess appropriate mechanical strength and swelling pressure, and concurrently support the proliferation of chondrocyte-like cells. The objective of this study was to develop and validate a composite hydrogel for NP tissue engineering, made of chitosan-poly(hydroxybutyrate-co-valerate) (CP) with chondroitin sulfate (CS) nanoparticles, without using a cross linker. The water uptake ability, as well as the viscoelastic properties of this composite hydrogel, was similar to native tissue, as reflected in the complex shear modulus and stress relaxation values. The hydrogel could withstand varying stress corresponding to daily activities like lying down (0.01 MPa), sitting (0.5 MPa) and standing (1.0 MPa) under dynamic conditions. The hydrogels were stable in PBS for 2 weeks and its stiffness, elastic and viscous modulus did not alter significantly during this period. Both CP and CP-CS hydrogels could assist the viability and adhesion of adipose derived rat mesenchymal stem cells (ADMSCs). The viability and chondrogenic differentiation of MSCs was significantly enhanced in presence of CS nanoparticles. Thus, CS nanoparticles-incorporated chitosan-PHBV hydrogels offer great potential for NP tissue engineering. Copyright © 2015 Elsevier B.V. All rights reserved.

High-purity production of ultrathin boron nitride nanosheets via shock chilling and their enhanced mechanical performance and transparency in nanocomposite hydrogels.

PubMed

Sun, Zemin; Lin, Liu; Yuan, Mengwei; Li, Huifeng; Sun, Genban; Ma, Shulan; Yang, Xiaojing

2018-05-25

A simple, highly efficient, and eco-friendly method is prepared to divide bulk boron nitride (BN) into boron nitride nanosheets (BNNSs). Due to the anisotropy of the hexagonal BN expansion coefficient, bulk BN is exfoliated utilizing the rapid and tremendous change in temperature, the extreme gasification of water, and ice thermal expansion pressure under freeze drying. The thickness of most of the BNNSs was less than ∼3 nm with a yield of 12-16 wt%. The as-obtained BNNS/polyacrylamide (PAAm) composite hydrogels exhibited outstanding mechanical properties. The tensile strength is fives times the bulk of the BN/PAAm composite hydrogels and the elongations are more than nine-fold the bulk of the BN/PAAm composite hydrogels. The BNNS/PAAm nanocomposite hydrogels also exhibited excellent elastic recovery, and the hysteresis of the BNNS nanocomposite hydrogels was negligible even after 30 cycles with a maximum tensile strain (ε max ) of 700%. This work provides new insight into the fabrication of BN/polymer nanocomposites utilizing the excellent mechanical properties and transparency of BN. The results confirm that a few layers of BNNSs can also efficiently and directly improve the mechanical properties of composite polymer due to its stronger surface free energy and better wettability.

Novel self-gelling injectable hydrogel/alpha-tricalcium phosphate composites for bone regeneration: Physiochemical and microcomputer tomographical characterization.

PubMed

Douglas, Timothy E L; Schietse, Josefien; Zima, Aneta; Gorodzha, Svetlana; Parakhonskiy, Bogdan V; KhaleNkow, Dmitry; Shkarin, Roman; Ivanova, Anna; Baumbach, Tilo; Weinhardt, Venera; Stevens, Christian V; Vanhoorne, Valérie; Vervaet, Chris; Balcaen, Lieve; Vanhaecke, Frank; Slośarczyk, Anna; Surmeneva, Maria A; Surmenev, Roman A; Skirtach, Andre G

2018-03-01

Mineralized hydrogels are increasingly gaining attention as biomaterials for bone regeneration. The most common mineralization strategy has been addition of preformed inorganic particles during hydrogel formation. This maintains injectability. One common form of bone cement is formed by mixing particles of the highly reactive calcium phosphate alpha-tricalcium phosphate (α-TCP) with water to form hydroxyapatite (HA). The calcium ions released during this reaction can be exploited to crosslink anionic, calcium-binding polymers such as the polysaccharide gellan gum (GG) to induce hydrogel formation. In this study, three different amounts of α-TCP particles were added to GG polymer solution to generate novel, injectable hydrogel-inorganic composites. Distribution of the inorganic phase in the hydrogel was studied by high resolution microcomputer tomography (µCT). Gelation occurred within 30 min. α-TCP converted to HA. µCT revealed inhomogeneous distribution of the inorganic phase in the composites. These results demonstrate the potential of the composites as alternatives to traditional α-TCP bone cement and pave the way for incorporation of biologically active substances and in vitro and in vivo testing. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 106A: 822-828, 2018. © 2017 Wiley Periodicals, Inc.

High-purity production of ultrathin boron nitride nanosheets via shock chilling and their enhanced mechanical performance and transparency in nanocomposite hydrogels

NASA Astrophysics Data System (ADS)

Sun, Zemin; Lin, Liu; Yuan, Mengwei; Li, Huifeng; Sun, Genban; Ma, Shulan; Yang, Xiaojing

2018-05-01

A simple, highly efficient, and eco-friendly method is prepared to divide bulk boron nitride (BN) into boron nitride nanosheets (BNNSs). Due to the anisotropy of the hexagonal BN expansion coefficient, bulk BN is exfoliated utilizing the rapid and tremendous change in temperature, the extreme gasification of water, and ice thermal expansion pressure under freeze drying. The thickness of most of the BNNSs was less than ∼3 nm with a yield of 12–16 wt%. The as-obtained BNNS/polyacrylamide (PAAm) composite hydrogels exhibited outstanding mechanical properties. The tensile strength is fives times the bulk of the BN/PAAm composite hydrogels and the elongations are more than nine-fold the bulk of the BN/PAAm composite hydrogels. The BNNS/PAAm nanocomposite hydrogels also exhibited excellent elastic recovery, and the hysteresis of the BNNS nanocomposite hydrogels was negligible even after 30 cycles with a maximum tensile strain (ε max) of 700%. This work provides new insight into the fabrication of BN/polymer nanocomposites utilizing the excellent mechanical properties and transparency of BN. The results confirm that a few layers of BNNSs can also efficiently and directly improve the mechanical properties of composite polymer due to its stronger surface free energy and better wettability.

Time-dependent chemo-electro-mechanical behavior of hydrogel-based structures

NASA Astrophysics Data System (ADS)

Leichsenring, Peter; Wallmersperger, Thomas

2018-03-01

Charged hydrogels are ionic polymer gels and belong to the class of smart materials. These gels are multiphasic materials which consist of a solid phase, a fluid phase and an ionic phase. Due to the presence of bound charges these materials are stimuli-responsive to electrical or chemical loads. The application of electrical or chemical stimuli as well as mechanical loads lead to a viscoelastic response. On the macroscopic scale, the response is governed by a local reversible release or absorption of water which, in turn, leads to a local decrease or increase of mass and a respective volume change. Furthermore, the chemo-electro-mechanical equilibrium of a hydrogel depends on the chemical composition of the gel and the surrounding solution bath. Due to the presence of bound charges in the hydrogel, this system can be understood as an osmotic cell where differences in the concentration of mobile ions in the gel and solution domain lead to an osmotic pressure difference. In the present work, a continuum-based numerical model is presented in order to describe the time-dependent swelling behavior of hydrogels. The numerical model is based on the Theory of Porous Media and captures the fluid-solid, fluid-ion and ion-ion interactions. As a direct consequence of the chemo-electro-mechanical equilibrium, the corresponding boundary conditions are defined following the equilibrium conditions. For the interaction of the hydrogel with surrounding mechanical structures, also respective jump condtions are formulated. Finaly, numerical results of the time-dependent behavior of a hydrogel-based chemo-sensor will be presented.

Living nano-micro fibrous woven fabric/hydrogel composite scaffolds for heart valve engineering.

PubMed

Wu, Shaohua; Duan, Bin; Qin, Xiaohong; Butcher, Jonathan T

2017-03-15

Regeneration and repair of injured or diseased heart valves remains a clinical challenge. Tissue engineering provides a promising treatment approach to facilitate living heart valve repair and regeneration. Three-dimensional (3D) biomimetic scaffolds that possess heterogeneous and anisotropic features that approximate those of native heart valve tissue are beneficial to the successful in vitro development of tissue engineered heart valves (TEHV). Here we report the development and characterization of a novel composite scaffold consisting of nano- and micro-scale fibrous woven fabrics and 3D hydrogels by using textile techniques combined with bioactive hydrogel formation. Embedded nano-micro fibrous scaffolds within hydrogel enhanced mechanical strength and physical structural anisotropy of the composite scaffold (similar to native aortic valve leaflets) and also reduced its compaction. We determined that the composite scaffolds supported the growth of human aortic valve interstitial cells (HAVIC), balanced the remodeling of heart valve ECM against shrinkage, and maintained better physiological fibroblastic phenotype in both normal and diseased HAVIC over single materials. These fabricated composite scaffolds enable the engineering of a living heart valve graft with improved anisotropic structure and tissue biomechanics important for maintaining valve cell phenotypes. Heart valve-related disease is an important clinical problem, with over 300,000 surgical repairs performed annually. Tissue engineering offers a promising strategy for heart valve repair and regeneration. In this study, we developed and tissue engineered living nano-micro fibrous woven fabric/hydrogel composite scaffolds by using textile technique combined with bioactive hydrogel formation. The novelty of our technique is that the composite scaffolds can mimic physical structure anisotropy and the mechanical strength of natural aortic valve leaflet. Moreover, the composite scaffolds prevented the matrix shrinkage, which is major problem that causes the failure of TEHV, and better maintained physiological fibroblastic phenotype in both normal and diseased HAVIC. This work marks the first report of a combination composite scaffold using 3D hydrogel enhanced by nano-micro fibrous woven fabric, and represents a promising tissue engineering strategy to treat heart valve injury. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Mechanically enhanced nested-network hydrogels as a coating material for biomedical devices.

PubMed

Wang, Zhengmu; Zhang, Hongbin; Chu, Axel J; Jackson, John; Lin, Karen; Lim, Chinten James; Lange, Dirk; Chiao, Mu

2018-04-01

Well-organized composite formations such as hierarchical nested-network (NN) structure in bone tissue and reticular connective tissue present remarkable mechanical strength and play a crucial role in achieving physical and biological functions for living organisms. Inspired by these delicate microstructures in nature, an analogous scaffold of double network hydrogel was fabricated by creating a poly(2-hydroxyethyl methacrylate) (pHEMA) network in the porous structure of alginate hydrogels. The resulting hydrogel possessed hierarchical NN structure and showed significantly improved mechanical strength but still maintained high elasticity comparable to soft tissues due to a mutual strengthening effect between the two networks. The tough hydrogel is also self-lubricated, exhibiting a surface friction coefficient comparable with polydimethylsiloxane (PDMS) substrates lubricated by a commercial aqueous lubricant (K-Y Jelly) and other low surface friction hydrogels. Additional properties of this hydrogel include high hydrophilicity, good biocompatibility, tunable cell adhesion and bacterial resistance after incorporation of silver nanoparticles. Firm bonding of the hydrogel on silicone substrates could be achieved through facile chemical modification, thus enabling the use of this hydrogel as a versatile coating material for biomedical applications. In this study, we developed a tough hydrogel by crosslinking HEMA monomers in alginate hydrogels and forming a well-organized structure of hierarchical nested network (NN). Different from most reported stretchable alginate-based hydrogels, the NN hydrogel shows higher compressive strength but retains comparable softness to alginate counterparts. This work further demonstrated the good integration of the tough hydrogel with silicone substrates through chemical modification and micropillar structures. Other properties including surface friction, biocompatibility and bacterial resistance were investigated and the hydrogel shows a great promise as a versatile coating material for biomedical applications. Copyright © 2018 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Gamma ray-induced synthesis of hyaluronic acid/chondroitin sulfate-based hydrogels for biomedical applications

NASA Astrophysics Data System (ADS)

Zhao, Linlin; Gwon, Hui-Jeong; Lim, Youn-Mook; Nho, Young-Chang; Kim, So Yeon

2015-01-01

Hyaluronic acid (HA)/chondroitin sulfate (CS)/poly(acrylic acid) (PAAc) hydrogel systems were synthesized by gamma-ray irradiation without the use of additional initiators or crosslinking agents to achieve a biocompatible hydrogel system for skin tissue engineering. HA and CS derivatives with polymerizable residues were synthesized. Then, the hydrogels composed of glycosaminoglycans, HA, CS, and a synthetic ionic polymer, PAAc, were prepared using gamma-ray irradiation through simultaneous free radical copolymerization and crosslinking. The physicochemical properties of the HA/CS/PAAc hydrogels having various compositions were investigated to evaluate their feasibility as artificial skin substitutes. The gel fractions of the HA/CS/PAAc hydrogels increased in absorbed doses up to 15 kGy, and they exhibited 91-93% gel fractions under 15 kGy radiation. All of the HA/CS/PAAc hydrogels exhibited relatively high water contents of over 90% and reached an equilibrium swelling state within 24 h. The enzymatic degradation kinetics of the HA/CS/PAAc hydrogels depended on both the concentration of the hyaluronidase solution and the ratio of HA/CS/PAAc. The in vitro drug release profiles of the HA/CS/PAAc hydrogels were significantly influenced by the interaction between the ionic groups in the hydrogels and the ionic drug molecules as well as the swelling of the hydrogels. From the cytotoxicity results of human keratinocyte (HaCaT) cells cultured with extracts of the HA/CS/PAAc hydrogels, all of the HA/CS/PAAc hydrogel samples tested showed relatively high cell viabilities of more than 82%, and did not induce any significant adverse effects on cell viability.

Biologically inspired rosette nanotubes and nanocrystalline hydroxyapatite hydrogel nanocomposites as improved bone substitutes

NASA Astrophysics Data System (ADS)

Zhang, Lijie; Rodriguez, Jose; Raez, Jose; Myles, Andrew J.; Fenniri, Hicham; Webster, Thomas J.

2009-04-01

Today, bone diseases such as bone fractures, osteoporosis and bone cancer represent a common and significant public health problem. The design of biomimetic bone tissue engineering materials that could restore and improve damaged bone tissues provides exciting opportunities to solve the numerous problems associated with traditional orthopedic implants. Therefore, the objective of this in vitro study was to create a biomimetic orthopedic hydrogel nanocomposite based on the self-assembly properties of helical rosette nanotubes (HRNs), the osteoconductive properties of nanocrystalline hydroxyapatite (HA), and the biocompatible properties of hydrogels (specifically, poly(2-hydroxyethyl methacrylate), pHEMA). HRNs are self-assembled nanomaterials that are formed from synthetic DNA base analogs in water to mimic the helical nanostructure of collagen in bone. In this study, different geometries of nanocrystalline HA were controlled by either hydrothermal or sintering methods. 2 and 10 wt% nanocrystalline HA particles were well dispersed into HRN hydrogels using ultrasonication. The nanocrystalline HA and nanocrystalline HA/HRN hydrogels were characterized by x-ray diffraction, transmission electron microscopy, and scanning electron microscopy. Mechanical testing studies revealed that the well dispersed nanocrystalline HA in HRN hydrogels possessed improved mechanical properties compared to hydrogel controls. In addition, the results of this study provided the first evidence that the combination of either 2 or 10 wt% nanocrystalline HA and 0.01 mg ml-1 HRNs in hydrogels greatly increased osteoblast (bone-forming cell) adhesion up to 236% compared to hydrogel controls. Moreover, this study showed that HRNs stimulated HA nucleation and mineralization along their main axis in a way that is very reminiscent of the HA/collagen assembly pattern in natural bone. In summary, the presently observed excellent properties of the biomimetic nanocrystalline HA/HRN hydrogel composites make them promising candidates for further study for bone tissue engineering applications.

Hydrogels That Allow and Facilitate Bone Repair, Remodeling, and Regeneration

PubMed Central

Short, Aaron R.; Koralla, Deepthi; Deshmukh, Ameya; Wissel, Benjamin; Stocker, Benjamin; Calhoun, Mark; Dean, David; Winter, Jessica O.

2015-01-01

Bone defects can originate from a variety of causes, including trauma, cancer, congenital deformity, and surgical reconstruction. Success of the current “gold standard” treatment (i.e., autologous bone grafts) is greatly influenced by insufficient or inappropriate bone stock. There is thus a critical need for the development of new, engineered materials for bone repair. This review describes the use of natural and synthetic hydrogels as scaffolds for bone tissue engineering. We discuss many of the advantages that hydrogels offer as bone repair materials, including their potential for osteoconductivity, biodegradability, controlled growth factor release, and cell encapsulation. We also discuss the use of hydrogels in composite devices with metals, ceramics, or polymers. These composites are useful because of the low mechanical moduli of hydrogels. Finally, the potential for thermosetting and photo-cross-linked hydrogels as three-dimensionally (3D) printed, patient-specific devices is highlighted. Three-dimensional printing enables controlled spatial distribution of scaffold materials, cells, and growth factors. Hydrogels, especially natural hydrogels present in bone matrix, have great potential to augment existing bone tissue engineering devices for the treatment of critical size bone defects. PMID:26693013

Hydrogels That Allow and Facilitate Bone Repair, Remodeling, and Regeneration.

PubMed

Short, Aaron R; Koralla, Deepthi; Deshmukh, Ameya; Wissel, Benjamin; Stocker, Benjamin; Calhoun, Mark; Dean, David; Winter, Jessica O

2015-10-28

Bone defects can originate from a variety of causes, including trauma, cancer, congenital deformity, and surgical reconstruction. Success of the current "gold standard" treatment (i.e., autologous bone grafts) is greatly influenced by insufficient or inappropriate bone stock. There is thus a critical need for the development of new, engineered materials for bone repair. This review describes the use of natural and synthetic hydrogels as scaffolds for bone tissue engineering. We discuss many of the advantages that hydrogels offer as bone repair materials, including their potential for osteoconductivity, biodegradability, controlled growth factor release, and cell encapsulation. We also discuss the use of hydrogels in composite devices with metals, ceramics, or polymers. These composites are useful because of the low mechanical moduli of hydrogels. Finally, the potential for thermosetting and photo-cross-linked hydrogels as three-dimensionally (3D) printed, patient-specific devices is highlighted. Three-dimensional printing enables controlled spatial distribution of scaffold materials, cells, and growth factors. Hydrogels, especially natural hydrogels present in bone matrix, have great potential to augment existing bone tissue engineering devices for the treatment of critical size bone defects.

Peripheral Nerve Repair in Rats Using Composite Hydrogel-Filled Aligned Nanofiber Conduits with Incorporated Nerve Growth Factor

PubMed Central

Jin, Jenny; Limburg, Sonja; Joshi, Sunil K.; Landman, Rebeccah; Park, Michelle; Zhang, Qia; Kim, Hubert T.

2013-01-01

Repair of peripheral nerve defects with current synthetic, tubular nerve conduits generally shows inferior recovery when compared with using nerve autografts, the current gold standard. We tested the ability of composite collagen and hyaluronan hydrogels, with and without the nerve growth factor (NGF), to stimulate neurite extension on a promising aligned, nanofiber poly-L-lactide-co-caprolactone (PLCL) scaffold. In vitro, the hydrogels significantly increased neurite extension from dorsal root ganglia explants. Consistent with these results, the addition of hydrogels as luminal fillers within aligned, nanofiber tubular PLCL conduits led to improved sensory function compared to autograft repair in a critical-size defect in the sciatic nerve in a rat model. Sensory recovery was assessed 3 and 12 weeks after repair using a withdrawal assay from thermal stimulation. The addition of hydrogel did not enhance recovery of motor function in the rat model. The NGF led to dose-dependent improvements in neurite out-growth in vitro, but did not have a significant effect in vivo. In summary, composite collagen/hyaluronan hydrogels enhanced sensory neurite outgrowth in vitro and sensory recovery in vivo. The use of such hydrogels as luminal fillers for tubular nerve conduits may therefore be useful in assisting restoration of protective sensation following peripheral nerve injury. PMID:23659607

Synthesized af-PFCl and GG-g-P(AN)/TEOS hydrogel composite used in hybridized technique applied for AMD treatment

NASA Astrophysics Data System (ADS)

Fosso-Kankeu, Elvis

2018-06-01

In the present study af-PFCl, GL-g-P(AN) hydrogel and GL-g-P(AN)/TEOS hydrogel composite were synthesized. The hydrogels were characterized using the fourier transformed infra-red (FTIR) and the scanning electron microscope (SEM) techniques. The coagulant af-PFCl and the hydrogels were applied consecutively in flocculation and adsorption processes respectively for the treatment of acid mine drainage (AMD). It was observed that the grafting process increased the amount of binding groups on the hydrogels. The hybridization of the techniques assisted in the removal of anions; while the cations were mostly removed by the adsorption process. The adsorbents behaviour was fittingly expressed by the pseudo-second order model. The adsorption capacities of GL-g-P(AN)/TEOS hydrogel composite for the removal of Al, As and Zn were 3.89, 0.66 and 0.394 respectively; while the adsorption capacities of GL-g-P(AN) for the removal of Al and Mg were 3.47 and 9.66 mg/g respectively. The techniques applied in this study have shown good potential for the removal of specific pollutants from the AMD; it is however, important that the appropriate hybridization of techniques allows to remove all the pollutants and restore acceptable water quality.

An Injectable Enzymatically Crosslinked Carboxymethylated Pullulan/Chondroitin Sulfate Hydrogel for Cartilage Tissue Engineering

PubMed Central

Chen, Feng; Yu, Songrui; Liu, Bing; Ni, Yunzhou; Yu, Chunyang; Su, Yue; Zhu, Xinyuan; Yu, Xiaowei; Zhou, Yongfeng; Yan, Deyue

2016-01-01

In this study, an enzymatically cross-linked injectable and biodegradable hydrogel system comprising carboxymethyl pullulan-tyramine (CMP-TA) and chondroitin sulfate-tyramine (CS-TA) conjugates was successfully developed under physiological conditions in the presence of both horseradish peroxidase (HRP) and hydrogen peroxide (H2O2) for cartilage tissue engineering (CTTE). The HRP crosslinking method makes this injectable system feasible, minimally invasive and easily translatable for regenerative medicine applications. The physicochemical properties of the mechanically stable hydrogel system can be modulated by varying the weight ratio and concentration of polymer as well as the concentrations of crosslinking reagents. Additionally, the cellular behaviour of porcine auricular chondrocytes encapsulated into CMP-TA/CS-TA hydrogels demonstrates that the hydrogel system has a good cyto-compatibility. Specifically, compared to the CMP-TA hydrogel, these CMP-TA/CS-TA composite hydrogels have enhanced cell proliferation and increased cartilaginous ECM deposition, which significantly facilitate chondrogenesis. Furthermore, histological analysis indicates that the hydrogel system exhibits acceptable tissue compatibility by using a mouse subcutaneous implantation model. Overall, the novel injectable pullulan/chondroitin sulfate composite hydrogels presented here are expected to be useful biomaterial scaffold for regenerating cartilage tissue. PMID:26817622

An Injectable Enzymatically Crosslinked Carboxymethylated Pullulan/Chondroitin Sulfate Hydrogel for Cartilage Tissue Engineering

NASA Astrophysics Data System (ADS)

Chen, Feng; Yu, Songrui; Liu, Bing; Ni, Yunzhou; Yu, Chunyang; Su, Yue; Zhu, Xinyuan; Yu, Xiaowei; Zhou, Yongfeng; Yan, Deyue

2016-01-01

In this study, an enzymatically cross-linked injectable and biodegradable hydrogel system comprising carboxymethyl pullulan-tyramine (CMP-TA) and chondroitin sulfate-tyramine (CS-TA) conjugates was successfully developed under physiological conditions in the presence of both horseradish peroxidase (HRP) and hydrogen peroxide (H2O2) for cartilage tissue engineering (CTTE). The HRP crosslinking method makes this injectable system feasible, minimally invasive and easily translatable for regenerative medicine applications. The physicochemical properties of the mechanically stable hydrogel system can be modulated by varying the weight ratio and concentration of polymer as well as the concentrations of crosslinking reagents. Additionally, the cellular behaviour of porcine auricular chondrocytes encapsulated into CMP-TA/CS-TA hydrogels demonstrates that the hydrogel system has a good cyto-compatibility. Specifically, compared to the CMP-TA hydrogel, these CMP-TA/CS-TA composite hydrogels have enhanced cell proliferation and increased cartilaginous ECM deposition, which significantly facilitate chondrogenesis. Furthermore, histological analysis indicates that the hydrogel system exhibits acceptable tissue compatibility by using a mouse subcutaneous implantation model. Overall, the novel injectable pullulan/chondroitin sulfate composite hydrogels presented here are expected to be useful biomaterial scaffold for regenerating cartilage tissue.

Gentamicin-Loaded Thermosetting Hydrogel and Moldable Composite Scaffold: Formulation Study and Biologic Evaluation.

PubMed

Dorati, Rossella; De Trizio, Antonella; Genta, Ida; Merelli, Alessia; Modena, Tiziana; Conti, Bice

2017-06-01

The aim was to design biodegradable drug delivery systems for gentamicin local delivery, meanwhile acting as scaffold for bone regeneration. Gentamicin-loaded thermosetting composite hydrogels were prepared combining chitosan with bovine bone substitutes (Orthoss® granules), beta-glycerophosphate as cross-linker, and lyophilized to obtain moldable composite scaffolds (moldable composite scaffold loaded with gentamicin [mCSG]). Diverse techniques for gentamicin loading into mCS were investigated by drug incorporation during hydrogel preparation or drug absorption on preformed mCS. Rheologic hydrogel characterization was performed. mCSGs were characterized for porosity, stability (water retention, water uptake), gentamicin release, cell seeding and proliferation, and antimicrobial effect on Escherichia coli ATCC 10356. Results show suitable gentamicin loadings were 4 mg in 1 mL thermosetting composite hydrogel starting solution, irreversible hydrogel thermosetting behavior, and cosolute effect of gentamicin on sol-gel transition. Positive results in terms of porosity (80%-86%), scaffold water uptake, and retention capability were obtained. Antibiotic in vitro release was completed in 4 h. Good cell seeding results were observed for mCSG1-5; mCSG3 and mCSG5 resulted the best as cell proliferation results. mCSG exerted bactericidal effect for 24 h, with superimposition of chitosan bacteriostatic effect in the first 4 h. The results lead to consider the drug delivery for reducing infection risk during bone open surgeries. Copyright © 2017 American Pharmacists Association®. Published by Elsevier Inc. All rights reserved.

Structuring and calorie control of bakery products by templating batter with ultra melt-resistant food-grade hydrogel beads.

PubMed

Thompson, Benjamin R; Horozov, Tommy S; Stoyanov, Simeon D; Paunov, Vesselin N

2017-08-01

We report the use of a temperature insensitive, food-grade hydrogel to reduce the caloric density of pancakes that were prepared at temperatures much higher than the boiling point of water. This cheap, facile method utilises a mixed agar-methylcellulose hydrogel, which was blended to produce a slurry of hydrogel microbeads. The pancake batter was mixed with a controlled volume percentage of slurry of hydrogel beads and cooked. From bomb calorimetry experiments, the composites were found to have a reduced caloric density that reflects the volume percentage of hydrogel beads mixed with the batter. Using this procedure, we were able to reduce the caloric density of pancakes by up to 23 ± 3% when the volume percentage of hydrogel beads initially used was 25%. The method is not limited to pancakes and could potentially be applied to various other food products. The structure and morphology of the freeze-dried pancakes and pancake-hydrogel composites were investigated and pores of a similar size to the hydrogel beads were found, confirming that the gel beads maintained their structure during the cooking process. There is scope for further development of this method by the encapsulation of nutritionally beneficial or flavour enhancing ingredients within the hydrogel beads.

Biomimetic hydrogels for biosensor implant biocompatibility: electrochemical characterization using micro-disc electrode arrays (MDEAs).

PubMed

Justin, Gusphyl; Finley, Stephen; Abdur Rahman, Abdur Rub; Guiseppi-Elie, Anthony

2009-02-01

Our interest is in the development of engineered microdevices for continuous remote monitoring of intramuscular lactate, glucose, pH and temperature during post-traumatic hemorrhaging. Two important design considerations in the development of such devices for in vivo diagnostics are discussed; the utility of micro-disc electrode arrays (MDEAs) for electrochemical biosensing and the application of biomimetic, bioactive poly(HEMA)-based hydrogel composites for implant biocompatibility. A poly(HEMA)-based hydrogel membrane containing polyethylene glycol (PEG) was UV cross-linked with tetraethyleneglycol diacrylate following application to MDEAs (50 mum discs) and to 250 mum diameter gold electrodes within 8-well culture ware. Cyclic voltammetry (CV) of the MDEAs revealed a reduction in the apparent diffusion coefficient of ferrocenemonocarboxylic acid (FcCO(2)H), from 6.68 x 10(-5) to 6.74 x 10(-6) cm(2)/s for the uncoated and 6 mum thick hydrogel coated devices, respectively. Single frequency (4 kHz) temporal impedance measurements of the hydrogels in the 8-well culture ware showed a reversible 5% change in the absolute impedance of the hydrogels when exposed to a pH change between 6.1 to 7.2 and a 20% drop between pH 6.1 and 8.8.

Influence of residual composition on the structure and properties of extracellular matrix derived hydrogels.

PubMed

Claudio-Rizo, Jesús A; Rangel-Argote, Magdalena; Castellano, Laura E; Delgado, Jorge; Mata-Mata, José L; Mendoza-Novelo, Birzabith

2017-10-01

In this work, hydrolysates of extracellular matrix (hECM) were obtained from rat tail tendon (TR), bovine Achilles tendon (TAB), porcine small intestinal submucosa (SIS) and bovine pericardium (PB), and they were polymerized to generate ECM hydrogels. The composition of hECM was evaluated by quantifying the content of sulphated glycosaminoglycans (sGAG), fibronectin and laminin. The polymerization process, structure, physicochemical properties, in vitro degradation and biocompatibility were studied and related to their composition. The results indicated that the hECM derived from SIS and PB were significantly richer in sGAG, fibronectin and laminin, than those derived from TAB and TR. These differences in hECM composition influenced the polymerization and the structural characteristics of the fibrillar gel network. Consequently, the swelling, mechanics and degradation of the hydrogels showed a direct relationship with the remaining composition. Moreover, the cytocompatibility and the secretion of transforming growth factor beta-1 (TGF-β1) by macrophages were enhanced in hydrogels with the highest residual content of ECM biomolecules. The results of this work evidenced the role of the ECM molecules remaining after both decellularization and hydrolysis steps to produce tissue derived hydrogels with structure and properties tailored to enhance their performance in tissue engineering and regenerative medicine applications. Copyright © 2017 Elsevier B.V. All rights reserved.

Ca:Mg:Zn:CO3 and Ca:Mg:CO3-tri- and bi-elemental carbonate microparticles for novel injectable self-gelling hydrogel-microparticle composites for tissue regeneration.

PubMed

Douglas, Timothy E L; Sobczyk, Katarzyna; Łapa, Agata; Włodarczyk, Katarzyna; Brackman, Gilles; Vidiasheva, Irina; Reczyńska, Katarzyna; Pietryga, Krzysztof; Schaubroeck, David; Bliznuk, Vitaliy; Voort, Pascal Van Der; Declercq, Heidi A; Bulcke, Jan Van den; Samal, Sangram Keshari; Khalenkow, Dmitry; Parakhonskiy, Bogdan V; Van Acker, Joris; Coenye, Tom; Lewandowska-Szumieł, Małgorzata; Pamuła, Elżbieta; Skirtach, Andre G

2017-03-24

Injectable composites for tissue regeneration can be developed by dispersion of inorganic microparticles and cells in a hydrogel phase. In this study, multifunctional carbonate microparticles containing different amounts of calcium, magnesium and zinc were mixed with solutions of gellan gum (GG), an anionic polysaccharide, to form injectable hydrogel-microparticle composites, containing Zn, Ca and Mg. Zn and Ca were incorporated into microparticle preparations to a greater extent than Mg. Microparticle groups were heterogeneous and contained microparticles of differing shape and elemental composition. Zn-rich microparticles were 'star shaped' and appeared to consist of small crystallites, while Zn-poor, Ca- and Mg-rich microparticles were irregular in shape and appeared to contain lager crystallites. Zn-free microparticle groups exhibited the best cytocompatibility and, unexpectedly, Zn-free composites showed the highest antibacterial activity towards methicilin-resistant Staphylococcus aureus. Composites containing Zn-free microparticles were cytocompatible and therefore appear most suitable for applications as an injectable biomaterial. This study proves the principle of creating bi- and tri-elemental microparticles to induce the gelation of GG to create injectable hydrogel-microparticle composites.

Removal of dye by carboxymethyl cellulose, acrylamide and graphene oxide via a free radical polymerization process.

PubMed

Varaprasad, Kokkarachedu; Jayaramudu, Tippabattini; Sadiku, Emmanuel Rotimi

2017-05-15

Carboxymethyl cellulose has been used for the design of novel engineered hydrogels in order to obtain effective three-dimensional structures for industrial applications. In this work, dye removal carboxymethyl cellulose-acrylamide-graphene oxide (CMC-AM-GO) hydrogels were prepared by a free-radical polymerization method. The GO was developed by the modified Hummers method. The CMC-AM-GO and GO were characterized by FTIR, XRD and SEM. The swelling and swelling kinetics were calculated using gravimetric process. The kinetic parameter, swelling exponent values [n=0.59-0.7507] explained the fact that the CMC-AM-GO hydrogles have super Case II diffusion transport mechanism. CMCx-AM-GO (x=1-4) and CMC-AM hydrogels were used for removal of Acid Blue-133. The result explains that composite hydrogels significantly removed the acid blue when compared to the neat hydrogel. The maximum AB absorption (185.45mg/g) capacity was found in the case of CMC 2 -AM-GO hydrogel. Therefore, cellulose-based GO hydrogels can be termed as smart systems for the abstraction of dye in water purification applications. Copyright © 2017 Elsevier Ltd. All rights reserved.

Radiation synthesis of poly[(dimethylaminoethyl methacrylate)-co-(ethyleneglycol dimethacrylate)] hydrogels and its application as a carrier for anticancer delivery

NASA Astrophysics Data System (ADS)

Mazied, Nabila A.; Ismail, Sahar A.; Abou Taleb, Manal F.

2009-11-01

The use of hydrogels as carriers for anticancer delivery has been a subject of significant recent research. In our recent work, we have shown that diffusion-controlled delivery of flutamide from hydrogels containing poly (dimethylaminoethyl methacrylate (DMAEMA)/ethyleneglycol dimethacrylate (EGDMA)) can be possible and controlled by the three-dimensional structure. Hydrogels based essentially on dimethylaminoethyl methacrylate and different ratios of ethyleneglycol dimethacrylate monomers were synthesized using gamma radiation copolymerization. The influence of copolymer composition and pH value of the surrounding medium on swelling behavior into the glassy polymer were discussed. The results showed that the ratio of EGDMA in the comonomer feeding solution has a great effect on the gel fraction and water content in the final hydrogel. In this regard, it was observed that the increase of EGDMA ratio decreased these properties. The ability of the prepared copolymer to be used as drug carrier for anticancer drug-delivery system was estimated using flutamide as a model drug. In vitro drug-release studies in different buffer solutions show that the basic parameters affecting the drug release behavior of hydrogel are the pH of the solution and DMAEMA content of hydrogel.

Biological oxygen demand in soils and hydrogel compositions for plant protection of the rhizosphere

NASA Astrophysics Data System (ADS)

Valentinovich Smagin, Andrey

2018-02-01

Potential biological activity of mineral and organogenic samples from light-textured sod-podzolic soils as well as of hydrogel compositions for protecting the root layer from pathogenic microflora and unfavorable edaphic factors were studied in laboratory conditions by oxygen consumption under the optimal hydrothermic conditions with portable gas analyzers. We have conducted ecological standardization of biological activity and organic matter destruction estimated by biological oxygen demand (BOD) in the widespread sandy soils. The primary outcome was the scale of gradations of biological oxygen uptake in soils with a range of quantities of potential biological activity from “very low” (<2 g·m-3·hour-1) to “extremely high” (>140 g·m-3·hour-1), obtained on the basis of statistical processing of data array 1308 measurements. Acrylic polymer hydrogels had BOD = 0.2-2 g·m-3·hour-1, which corresponded to the periods of their half-lives from 0.2±0.1 to 6.8± 4.5 years, or relatively low resistance to biodestruction. In contrast to the pure gels, hydrogel compositions for rhizosphere based on ionic and colloidal silver showed low biological activity (BOD=0.01-0.2 g·m-3· hour-1) and, accordingly, significant resistance to biodegradation with half-lives from 5 to 70 years and above.

Mechanomimetic hydrogels for vocal fold lamina propria regeneration.

PubMed

Kutty, Jaishankar K; Webb, Ken

2009-01-01

Vocal fold injury commonly leads to reduced vocal quality due to scarring-induced alterations in matrix composition and tissue biomechanics. The long-term hypothesis motivating our work is that rapid restoration of phonation and the associated dynamic mechanical environment will reduce scarring and promote regenerative healing. Toward this end, the objective of this study was to develop mechanomimetic, degradable hydrogels approximating the viscoelastic properties of the vocal ligament and mucosa that may be photopolymerized in situ to restore structural integrity to vocal fold tissues. The tensile and rheological properties of hydrogels (targeting the vocal ligament and mucosa, respectively) were varied as a function of macromer concentration. PEG diacrylate-based hydrogels exhibited linear stress-strain response and elastic modulus consistent with the properties of the vocal ligament at low strains (0-15%), but did not replicate the non-linear behavior observed in native tissue at higher strains. Methacrylated hyaluronic acid hydrogels displayed dynamic viscosity consistent with native vocal mucosa, while elastic shear moduli values were several-fold higher. Cell culture studies indicated that both hydrogels supported spreading, proliferation and collagen/proteoglycan matrix deposition by encapsulated fibroblasts throughout the 3D network.

Silk-ionomer and silk-tropoelastin hydrogels as charged three-dimensional culture platforms for the regulation of hMSC response.

PubMed

Calabrese, Rossella; Raia, Nicole; Huang, Wenwen; Ghezzi, Chiara E; Simon, Marc; Staii, Cristian; Weiss, Anthony S; Kaplan, David L

2017-09-01

The response of human bone marrow-derived mesenchymal stem cells (hMSCs) encapsulated in three-dimensional (3D) charged protein hydrogels was studied. Combining silk fibroin (S) with recombinant human tropoelastin (E) or silk ionomers (I) provided protein composite alloys with tunable physicochemical and biological features for regulating the bioactivity of encapsulated hMSCs. The effects of the biomaterial charges on hMSC viability, proliferation and chondrogenic or osteogenic differentiation were assessed. The silk-tropoelastin or silk-ionomers hydrogels supported hMSC viability, proliferation and differentiation. Gene expression of markers for chondrogenesis and osteogenesis, as well as biochemical and histological analysis, showed that hydrogels with different S/E and S/I ratios had different effects on cell fate. The negatively charged hydrogels upregulated hMSC chondrogenesis or osteogenesis, with or without specific differentiation media, and hydrogels with higher tropoelastin content inhibited the differentiation potential even in the presence of the differentiation media. The results provide insight on charge-tunable features of protein-based biomaterials to control hMSC differentiation in 3D hydrogels, as well as providing a new set of hydrogels for the compatible encapsulation and utility for cell functions. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

Interwoven Aligned Conductive Nanofiber Yarn/Hydrogel Composite Scaffolds for Engineered 3D Cardiac Anisotropy.

PubMed

Wu, Yaobin; Wang, Ling; Guo, Baolin; Ma, Peter X

2017-06-27

Mimicking the anisotropic cardiac structure and guiding 3D cellular orientation play a critical role in designing scaffolds for cardiac tissue regeneration. Significant advances have been achieved to control cellular alignment and elongation, but it remains an ongoing challenge for engineering 3D cardiac anisotropy using these approaches. Here, we present a 3D hybrid scaffold based on aligned conductive nanofiber yarns network (NFYs-NET, composition: polycaprolactone, silk fibroin, and carbon nanotubes) within a hydrogel shell for mimicking the native cardiac tissue structure, and further demonstrate their great potential for engineering 3D cardiac anisotropy for cardiac tissue engineering. The NFYs-NET structures are shown to control cellular orientation and enhance cardiomyocytes (CMs) maturation. 3D hybrid scaffolds were then fabricated by encapsulating NFYs-NET layers within hydrogel shell, and these 3D scaffolds performed the ability to promote aligned and elongated CMs maturation on each layer and individually control cellular orientation on different layers in a 3D environment. Furthermore, endothelialized myocardium was constructed by using this hybrid strategy via the coculture of CMs on NFYs-NET layer and endothelial cells within hydrogel shell. Therefore, these 3D hybrid scaffolds, containing NFYs-NET layer inducing cellular orientation, maturation, and anisotropy and hydrogel shell providing a suitable 3D environment for endothelialization, has great potential in engineering 3D cardiac anisotropy.

[Studies of local anaesthetics - part 197. Effect of xylitol on pharmaceutical availability of lidocaine and flow properties of hydrogels].

PubMed

Zuzana, Vitková; Petra, Herdová; Jozef, Cižmárik; Daniel, Grančai; Lukáš, Benč

2012-06-01

The paper examines the formulation of hydrogel on the base of a synthetic polymer containing a local anaesthetic and a mass-produced drug in the form of a solution with an antiphlogistic effect. It aimed to prepare a hydrogel of a suitable composition with suitable flow properties and drug release, the active ingredient being lidocaine hydrochloride. Besides the role of a synthetic polymer which ensures that the active ingredient remains at the affected site, an important role in the formulation is played by the presence of an artificial sweetener, which to a great extent as a taste correcting agent of the unpleasant taste of the active ingredient influences the compliance of many patients. The study examined the effect of concentration of the artificial sweetener xylitol on the liberation of the active ingredient from prepared hydrogels. The optimum concentration of the artificial sweetener was adjusted to a degree which does not affect the qualitative properties of the active ingredient. lidocaine hydrochloride, xylitol, hydrogel, liberation.

In Situ Mineralization of Magnetite Nanoparticles in Chitosan Hydrogel

NASA Astrophysics Data System (ADS)

Wang, Yongliang; Li, Baoqiang; Zhou, Yu; Jia, Dechang

2009-09-01

Based on chelation effect between iron ions and amino groups of chitosan, in situ mineralization of magnetite nanoparticles in chitosan hydrogel under ambient conditions was proposed. The chelation effect between iron ions and amino groups in CS-Fe complex, which led to that chitosan hydrogel exerted a crucial control on the magnetite mineralization, was proved by X-ray photoelectron spectrum. The composition, morphology and size of the mineralized magnetite nanoparticles were characterized by X-ray diffraction, Raman spectroscopy, transmission electron microscopy and thermal gravity. The mineralized nanoparticles were nonstoichiometric magnetite with a unit formula of Fe2.85O4 and coated by a thin layer of chitosan. The mineralized magnetite nanoparticles with mean diameter of 13 nm dispersed in chitosan hydrogel uniformly. Magnetization measurement indicated that superparamagnetism behavior was exhibited. These magnetite nanoparticles mineralized in chitosan hydrogel have potential applications in the field of biotechnology. Moreover, this method can also be used to synthesize other kinds of inorganic nanoparticles, such as ZnO, Fe2O3 and hydroxyapatite.

P(4-vinyl pyridine) hydrogel use for the removal of UO(2)(2+) and Th(4+) from aqueous environments.

PubMed

Ozay, Ozgur; Ekici, Sema; Aktas, Nahit; Sahiner, Nurettin

2011-12-01

4-vinyl pyridine (4-VP) based hydrogels with 2-hydroxyethylmetacrylate (HEMA) and magnetic composites were prepared and tested for use in the removal of UO(2)(2+) and Th(4+) ions from aqueous environments. It was found that the absorption of these metal ions from aqueous environments decreased with an increase in the amount of HEMA contained within p(4-VP-co-HEMA) hydrogels between 0.498 mmol for pure p(4-VP) and 0.027 mmol for pure p(HEMA). The characterization of the hydrogels was determined by swelling experiments, FT-IR and thermal analysis. The effects of initial metal ion concentration, hydrogel amount and the temperature of the medium on absorption of the ions were investigated. Langmuir and Freundlich isotherms were constructed for the absorption of UO(2)(2+) and Th(4+). Both isotherms demonstrated that these metal ions complied with monolayer absorption kinetics. Copyright © 2011 Elsevier Ltd. All rights reserved.

Release behavior and bioefficacy of imazethapyr formulations based on biopolymeric hydrogels.

PubMed

Kumar, Vikas; Singh, Anupama; Das, T K; Sarkar, Dhruba Jyoti; Singh, Shashi Bala; Dhaka, Rashmi; Kumar, Anil

2017-06-03

Controlled release formulations of imazethapyr herbicide have been developed employing guar gum-g-cl-polyacrylate/bentonite clay hydrogel composite (GG-HG) and guar gum-g-cl-PNIPAm nano hydrogel (GG-NHG) as carriers, to assess the suitability of biopolymeric hydrogels as controlled herbicide release devices. The kinetics of imazethapyr release from the developed formulations was studied in water and it revealed that the developed formulations of imazethapyr behaved as slow release formulations as compared to commercial formulation. The calculated diffusion exponent (n) values showed that Fickian diffusion was the predominant mechanism of imazethapyr release from the developed formulations. Time for release of half of the loaded imazethapyr (t 1/2 ) ranged between 0.06 and 4.8 days in case of GG-NHG and 4.4 and 12.6 days for the GG-HG formulations. Weed control index (WCI) of GG-HG and GG-NHG formulations was similar to that of the commercial formulation and the herbicidal effect was observed for relatively longer period. Guar gum-based biopolymeric hydrogels in both macro and nano particle size range can serve as potential carriers in developing slow release herbicide formulations.

Formulation Changes Affect Material Properties and Cell Behavior in HA-Based Hydrogels.

PubMed

Lawyer, Thomas; McIntosh, Kristen; Clavijo, Cristian; Potekhina, Lydia; Mann, Brenda K

2012-01-01

To develop and optimize new scaffold materials for tissue engineering applications, it is important to understand how changes to the scaffold affect the cells that will interact with that scaffold. In this study, we used a hyaluronic acid- (HA-) based hydrogel as a synthetic extracellular matrix, containing modified HA (CMHA-S), modified gelatin (Gtn-S), and a crosslinker (PEGda). By varying the concentrations of these components, we were able to change the gelation time, enzymatic degradation, and compressive modulus of the hydrogel. These changes also affected fibroblast spreading within the hydrogels and differentially affected the proliferation and metabolic activity of fibroblasts and mesenchymal stem cells (MSCs). In particular, PEGda concentration had the greatest influence on gelation time, compressive modulus, and cell spreading. MSCs appeared to require a longer period of adjustment to the new microenvironment of the hydrogels than fibroblasts. Fibroblasts were able to proliferate in all formulations over the course of two weeks, but MSCs did not. Metabolic activity changed for each cell type during the two weeks depending on the formulation. These results highlight the importance of determining the effect of matrix composition changes on a particular cell type of interest in order to optimize the formulation for a given application.

One-pot synthesis and lubricity of fluorescent carbon dots applied on PCL-PEG-PCL hydrogel.

PubMed

Guo, Junde; Mei, Tangjie; Li, Yue; Hafezi, Mahshid; Lu, Hailin; Li, Jianhui; Dong, Guangneng

2018-06-12

This work presents a method for one-pot synthesis of N-doped nanometer-size carbon dots, which can be assembled with thermosensitive poly(ε-caprolactone)-poly(ethylene glycol)-poly(ε-caprolactone) (PCL-PEG-PCL, PCEC) hydrogel to achieve slow-release lubricity. The typical property of this green production was studied by fourier transform infrared (FT-IR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscope (TEM). The photoluminescence of composite PCEC/CDs hydrogel and its released solutions were characterized by ultraviolet spectrum, and the rheological properties were tested by rotary rheometer. Tribological performance of the released solution from composite PCEC/CDs hydrogel was obtained to compare with PBS and pure CDs solution. The experimental results reveal that the CDs contain the chemical groups of N-H, C-OH/C-O-C and -COOH, etc. In addition, the diameter of the CDs is in the range of 6~8 nm. The phase transition behavior of PCEC/CDs hydrogel can be still kept and its viscoelasticity hydrogel is improved by approximatively 7%. Furthermore, friction coefficient of the released solution from composite PCEC/CDs hydrogel decreases by about 70% than that of PBS. Besides, the wear condition can be improved by a lubricating transfer film formed by released CDs. This novel strategy for slow-release application is valuable for drug delivery and bio-tribology.

A shape memory foam composite with enhanced fluid uptake and bactericidal properties as a hemostatic agent.

PubMed

Landsman, T L; Touchet, T; Hasan, S M; Smith, C; Russell, B; Rivera, J; Maitland, D J; Cosgriff-Hernandez, E

2017-01-01

Uncontrolled hemorrhage accounts for more than 30% of trauma deaths worldwide. Current hemostatic devices focus primarily on time to hemostasis, but prevention of bacterial infection is also critical for improving survival rates. In this study, we sought to improve on current devices used for hemorrhage control by combining the large volume-filling capabilities and rapid clotting of shape memory polymer (SMP) foams with the swelling capacity of hydrogels. In addition, a hydrogel composition was selected that readily complexes with elemental iodine to impart bactericidal properties to the device. The focus of this work was to verify that the advantages of each respective material (SMP foam and hydrogel) are retained when combined in a composite device. The iodine-doped hydrogel demonstrated an 80% reduction in bacteria viability when cultured with a high bioburden of Staphylococcus aureus. Hydrogel coating of the SMP foam increased fluid uptake by 19× over the uncoated SMP foam. The composite device retained the shape memory behavior of the foam with more than 15× volume expansion after being submerged in 37°C water for 15 min. Finally, the expansion force of the composite was tested to assess potential tissue damage within the wound during device expansion. Expansion forces did not exceed 0.6N, making tissue damage during device expansion unlikely, even when the expanded device diameter is substantially larger than the target wound site. Overall, the enhanced fluid uptake and bactericidal properties of the shape memory foam composite indicate its strong potential as a hemostatic agent to treat non-compressible wounds. No hemostatic device currently used in civilian and combat trauma situations satisfies all the desired criteria for an optimal hemostatic wound dressing. The research presented here sought to improve on current devices by combining the large volume-filling capabilities and rapid clotting of shape memory polymer (SMP) foams with the swelling capacity of hydrogels. In addition, a hydrogel composition was selected that readily complexes with elemental iodine to impart bactericidal properties to the device. The focus of this work was to verify that the advantages of each respective material are retained when combined into a composite device. This research opens the door to generating novel composites with a focus on both hemostasis, as well as wound healing and microbial prevention. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Rheological behavior and Ibuprofen delivery applications of pH responsive composite alginate hydrogels.

PubMed

Jabeen, Suraya; Maswal, Masrat; Chat, Oyais Ahmad; Rather, Ghulam Mohammad; Dar, Aijaz Ahmad

2016-03-01

Synthesis and structural characterization of hydrogels composed of sodium alginate, polyethylene oxide and acrylic acid with cyclodextrin as the hydrocolloid prepared at different pH values is presented. The hydrogels synthesized show significant variations in rheological properties, drug encapsulation capability and release kinetics. The hydrogels prepared at lower pH (pH 1) are more elastic, have high tensile strength and remain almost unaffected by varying temperature or frequency. Further, their Ibuprofen encapsulation capacity is low and releases it slowly. The hydrogel prepared at neutral pH (pH 7) is viscoelastic, thermo-reversible and also exhibits sol-gel transition on applying frequency and changing temperature. It shows highest Ibuprofen encapsulation capacity and also optimum drug release kinetics. The hydrogel prepared at higher pH (pH 12) is more viscous, has low tensile strength, is unstable to change in temperature and has fast drug release rate. The study highlights the pH responsiveness of three composite alginate hydrogels prepared under different conditions to be employed in drug delivery applications. Copyright © 2015 Elsevier B.V. All rights reserved.

Drug loading optimization and extended drug delivery of corticoids from pHEMA based soft contact lenses hydrogels via chemical and microstructural modifications.

PubMed

García-Millán, Eva; Koprivnik, Sandra; Otero-Espinar, Francisco Javier

2015-06-20

This paper proposes an approach to improve drug loading capacity and release properties of poly(2-hydroxyethyl methacrylate) (p(HEMA)) soft contact lenses based on the optimization of the hydrogel composition and microstructural modifications using water during the polymerization process. P(HEMA) based soft contact lenses were prepared by thermal or photopolymerization of 2-hydroxyethyl methacrylate (HEMA) solutions containing ethylene glycol di-methacrylate as crosslinker and different proportions of N-vinyl-2-pyrrolidone (NVP) or methacrylic acid (MA) as co-monomers. Transmittance, water uptake, swelling, microstructure, drug absorption isotherms and in vitro release were characterized using triamcinolone acetonide (TA) as model drug. Best drug loading ratios were obtained with lenses containing the highest amount (200 mM) of MA. Incorporation of 40% V/V of water during the polymerization increases the hydrogel porosity giving a better drug loading capacity. In vitro TA release kinetics shows that MA hydrogels released the drug significantly faster than NVP-hydrogels. Drug release was found to be diffusion controlled and kinetics was shown to be reproducible after consecutive drug loading/release processes. Results of p(HEMA) based soft contact lenses copolymerized with ethylene glycol dimethacrylate (EGDMA) and different co-monomers could be a good alternative to optimize the loading and ocular drug delivery of this corticosteroid drug. Copyright © 2015. Published by Elsevier B.V.

Preparation of monodisperse PEG hydrogel composite microspheres via microfluidic chip with rounded channels

NASA Astrophysics Data System (ADS)

Yu, Bing; Cong, Hailin; Liu, Xuesong; Ren, Yumin; Wang, Jilei; Zhang, Lixin; Tang, Jianguo; Ma, Yurong; Akasaka, Takeshi

2013-09-01

An effective microfluidic method to fabricate monodisperse polyethylene glycol (PEG) hydrogel composite microspheres with tunable dimensions and properties is reported in this paper. A T-junction microfluidic chip equipped with rounded channels and online photopolymerization system is applied for the microsphere microfabrication. The shape and size of the microspheres are well controlled by the rounded channels and PEG prepolymer/silicon oil flow rate ratios. The obtained PEG/aspirin composite microspheres exhibit a sustained release of aspirin for a wide time range; the obtained PEG/Fe3O4 nanocomposite microspheres exhibit excellent magnetic properties; and the obtained binary PEG/dye composite microspheres show the ability to synchronously load two functional components in the same peanut-shaped or Janus hydrogel particles.

Influence of clay particles on microfluidic-based preparation of hydrogel composite microsphere

NASA Astrophysics Data System (ADS)

Hong, Joung Sook

2016-05-01

For the successful fabrication of a hydrogel composite microsphere, this study aimed to investigate the influence of clay particles on microsphere formation in a microfluidic device which has flow focusing and a 4.5:1 contraction channel. A poly alginic acid solution (2.0 wt.%) with clay particles was used as the dispersed phase to generate drops in an oil medium, which then merged with drops of a CaCl2 solution for gelation. Drop generations were observed with different flow rates and particles types. When the flow rate increased, drop generation was enhanced and drop size decreased by the build-up of more favorable hydrodynamic flow conditions to detach the droplets. The addition of a small amount of particles insignificantly changed the drop generation behavior even though it reduced interfacial tension and increased the viscosity of the solution. Instead, clays particles significantly affected hydro-gelation depending on the hydrophobicity of particles, which produced further heterogeneity in the shape and size of microsphere.

Nanoparticle-Hydrogel Composites: Concept, Design, and Applications of These Promising, Multi-Functional Materials.

PubMed

Thoniyot, Praveen; Tan, Mein Jin; Karim, Anis Abdul; Young, David James; Loh, Xian Jun

2015-02-01

New technologies rely on the development of new materials, and these may simply be the innovative combination of known components. The structural combination of a polymer hydrogel network with a nanoparticle (metals, non-metals, metal oxides, and polymeric moieties) holds the promise of providing superior functionality to the composite material with applications in diverse fields, including catalysis, electronics, bio-sensing, drug delivery, nano-medicine, and environmental remediation. This mixing may result in a synergistic property enhancement of each component: for example, the mechanical strength of the hydrogel and concomitantly decrease aggregation of the nanoparticles. These mutual benefits and the associated potential applications have seen a surge of interest in the past decade from multi-disciplinary research groups. Recent advances in nanoparticle-hydrogel composites are herein reviewed with a focus on their synthesis, design, potential applications, and the inherent challenges accompanying these exciting materials.

Nanoparticle–Hydrogel Composites: Concept, Design, and Applications of These Promising, Multi‐Functional Materials

PubMed Central

Thoniyot, Praveen; Tan, Mein Jin; Karim, Anis Abdul; Young, David James

2015-01-01

New technologies rely on the development of new materials, and these may simply be the innovative combination of known components. The structural combination of a polymer hydrogel network with a nanoparticle (metals, non‐metals, metal oxides, and polymeric moieties) holds the promise of providing superior functionality to the composite material with applications in diverse fields, including catalysis, electronics, bio‐sensing, drug delivery, nano‐medicine, and environmental remediation. This mixing may result in a synergistic property enhancement of each component: for example, the mechanical strength of the hydrogel and concomitantly decrease aggregation of the nanoparticles. These mutual benefits and the associated potential applications have seen a surge of interest in the past decade from multi‐disciplinary research groups. Recent advances in nanoparticle–hydrogel composites are herein reviewed with a focus on their synthesis, design, potential applications, and the inherent challenges accompanying these exciting materials. PMID:27980900

Rheological study of in-situ crosslinkable hydrogels based on hyaluronanic acid, collagen and sericin.

PubMed

Vulpe, Raluca; Le Cerf, Didier; Dulong, Virginie; Popa, Marcel; Peptu, Catalina; Verestiuc, Liliana; Picton, Luc

2016-12-01

The elaboration of chemically crosslinked hydrogels based on collagen (C), hyaluronanic acid (HA) and sericin (S) with different polymer ratios was investigated by in-situ rheology. This reaction was performed via amide or ester bond reaction activated by carbodiimide, in pure water. Prior to molecule crosslinking, the rheological behaviour of the biopolymers (alone or in mixture) was characterized in a semi-dilute concentration regime. Both flow and dynamic measurements showed that uncrosslinked collagen alone appears to be rather elastic with yield stress properties, whereas uncrosslinked HA alone appears to be rather shear thinning and viscoelastic in agreement with entangled polymer behaviour. Sericin exhibited Newtonian low viscosity behaviour according to its very low molar mass. Before crosslinking, HA exhibited viscoelastic behaviour at concentrations above the critical entangled concentration (C*) in the mixtures, thus HA shows promise as a matrix for future crosslinked networks, whereas sericin did not significantly modify the rheology. During the reaction, followed by rheology, the kinetics were slower for pure HA systems compared with the mixtures (i.e., with added collagen and/or to a lesser extent sericin). At the same time, the final network of hydrogels (i.e., the elastic modulus) was more structured in the mixture based systems. This result is explained by ester bonds (the only possibility for pure HA systems), which are less favourable and reactive than amide bonds (possible with sericin and collagen). The presence of collagen in the HA matrix reinforced the hydrogel network. SEM studies confirmed the structure of the hydrogels, and in vitro degradability was globally consistent with the effect of the selected enzyme according to the hydrogel composition. All the elaborated hydrogels were non-cytotoxic in vitro. Copyright © 2016 Elsevier B.V. All rights reserved.

A 3D tension bioreactor platform to study the interplay between ECM stiffness and tumor phenotype.

PubMed

Cassereau, Luke; Miroshnikova, Yekaterina A; Ou, Guanqing; Lakins, Johnathon; Weaver, Valerie M

2015-01-10

Extracellular matrix (ECM) structure, composition, and stiffness have profound effects on tissue development and pathologies such as cardiovascular disease and cancer. Accordingly, a variety of synthetic hydrogel systems have been designed to study the impact of ECM composition, density, mechanics, and topography on cell and tissue phenotype. However, these synthetic systems fail to accurately recapitulate the biological properties and structure of the native tissue ECM. Natural three dimensional (3D) ECM hydrogels, such as collagen or hyaluronic acid, feature many of the chemical and physical properties of tissue, yet, these systems have limitations including the inability to independently control biophysical properties such as stiffness and pore size. Here, we present a 3D tension bioreactor system that permits precise mechanical tuning of collagen hydrogel stiffness, while maintaining consistent composition and pore size. We achieve this by mechanically loading collagen hydrogels covalently-conjugated to a polydimethylsiloxane (PDMS) membrane to induce hydrogel stiffening. We validated the biological application of this system with oncogenically transformed mammary epithelial cell organoids embedded in a 3D collagen I hydrogel, either uniformly stiffened or calibrated to create a gradient of ECM stiffening, to visually demonstrate the impact of ECM stiffening on transformation and tumor cell invasion. As such, this bioreactor presents the first tunable 3D natural hydrogel system that is capable of independently assessing the role of ECM stiffness on tissue phenotype. Copyright © 2014 Elsevier B.V. All rights reserved.

A multiple phase transitioning peptide hydrogel for use in vascular a | NCI Technology Transfer Center | TTC

Cancer.gov

Researchers at the National Cancer Institute (NCI), in collaboration with surgical specialists from Johns Hopkins University, have developed hydrogel compositions and methods to suture blood vessels with the hydrogels during microsurgery. These hydrogels are particularly beneficial for surgeons in whole tissue transplant procedures. The NCI researchers seek licensing and/or co-development research collaborations for further development of this technology.

Fabrication of hydrogel-coated single conical nanochannels exhibiting controllable ion rectification characteristics.

PubMed

Wang, Linlin; Zhang, Huacheng; Yang, Zhe; Zhou, Jianjun; Wen, Liping; Li, Lin; Jiang, Lei

2015-03-07

Heterogeneous nanochannel materials that endow new functionalities different to the intrinsic properties of two original nanoporous materials have wide potential applications in nanofluidics, energy conversion, and biosensors. Herein, we report novel, interesting hydrogel-composited nanochannel devices with regulatable ion rectification characteristics. The heterogeneous nanochannel devices were constructed by selectively coating the tip side, base side, or both sides of a single conical nanochannel membrane with thin agar hydrogel layers. The tunable ion current rectification of the nanochannels in the three different coating states was systematically demonstrated by current-voltage (I-V) curves. The asymmetric ionic transport property of the conical nanochannel was further strengthened in the tip-coating state and weakened in the base-coating state, whereas the conical nanochannel showed nearly symmetric ionic transport in the dual-coating state. Repeated experiments presented insight into the good stability and reversibility of the three coating states of the hydrogel-nanochannel-integrated systems. This work, as an example, may provide a new strategy to further design and develop multifunctional gel-nanochannel heterogeneous smart porous nanomaterials.

Morphological Characterization of Silicone Hydrogels

NASA Astrophysics Data System (ADS)

Gido, Samuel

2007-03-01

Silicone hydrogel materials are used in the latest generation of extended wear soft contact lenses. To ensure comfort and eye health, these materials must simultaneously exhibit high oxygen permeability and high water permeability / hydrophilicity. The materials achieve these opposing requirements based on bicontinuous composite of nanoscale domains of oxygen permeable (silicones) and hydrophilic (water soluble polymer) materials. The microphase separated morphology of silicone hydrogel contact lens materials was imaged using field emission gun scanning transmission electron microscopy (FEGSTEM), and atomic force microscopy (AFM). Additional morphological information was provided by small angle X-ray scattering (SAXS). These results all indicate a nanophase separated structure of silicone rich (oxygen permeable) and carbon rich (water soluble polymer) domains separated on a length scale of about 10 nm.

Three-dimensional design and fabrication of reduced graphene oxide/polyaniline composite hydrogel electrodes for high performance electrochemical supercapacitors

NASA Astrophysics Data System (ADS)

Ates, Murat; El-Kady, Maher; Kaner, Richard B.

2018-04-01

Graphene/polyaniline composite hydrogels (GH/PANI) were chemically synthesized by in situ polymerization of aniline monomer. Graphene hydrogels were obtained by a hydrothermal method and used in supercapacitors. The graphene/polyaniline composite hydrogel exhibits better electrochemical performance than the pure individual components as determined by cyclic voltammetry (CV), galvanostatic charge-discharge (GCD), and electrochemical impedance spectroscopic measurements. A remarkable specific capacitance (C sp) of 323.9 F g-1 was measured using CV at a scan rate of 2 mV s-1 at 25 °C. GCD measurements (311.3 F g-1) and electrochemical impedance analysis also support these results. The numbers were obtained at extremely high loading masses: 7.14 mg cm-2 for GH and GH/PANI synthesized at 0 °C, and 8.93 mg cm-2 for GH/PANI synthesized at 25 °C. The corresponding areal capacitances are 1.14, 1.75 and 2.78 F cm-2 for GH, and GH/PANI composite hydrogels synthesized at 0 °C and 25 °C, respectively. These values in F cm-2 are 3.80, 5.83 and 9.27 times higher than commercially available activated carbon supercapacitors (˜0.3 F cm-2 for a two electrode system). Moreover, the GH/PANI composite synthesized at 25 °C exhibits excellent stability with 99% initial capacitance retention after 1000 charge/discharge cycles. GH/PANI composites synthesized at 0 °C and 25 °C therefore hold promise for use in supercapacitor device applications.

Three-dimensional design and fabrication of reduced graphene oxide/polyaniline composite hydrogel electrodes for high performance electrochemical supercapacitors.

PubMed

Ates, Murat; El-Kady, Maher; Kaner, Richard B

2018-04-27

Graphene/polyaniline composite hydrogels (GH/PANI) were chemically synthesized by in situ polymerization of aniline monomer. Graphene hydrogels were obtained by a hydrothermal method and used in supercapacitors. The graphene/polyaniline composite hydrogel exhibits better electrochemical performance than the pure individual components as determined by cyclic voltammetry (CV), galvanostatic charge-discharge (GCD), and electrochemical impedance spectroscopic measurements. A remarkable specific capacitance (C sp ) of 323.9 F g -1 was measured using CV at a scan rate of 2 mV s -1 at 25 °C. GCD measurements (311.3 F g -1 ) and electrochemical impedance analysis also support these results. The numbers were obtained at extremely high loading masses: 7.14 mg cm -2 for GH and GH/PANI synthesized at 0 °C, and 8.93 mg cm -2 for GH/PANI synthesized at 25 °C. The corresponding areal capacitances are 1.14, 1.75 and 2.78 F cm -2 for GH, and GH/PANI composite hydrogels synthesized at 0 °C and 25 °C, respectively. These values in F cm -2 are 3.80, 5.83 and 9.27 times higher than commercially available activated carbon supercapacitors (∼0.3 F cm -2 for a two electrode system). Moreover, the GH/PANI composite synthesized at 25 °C exhibits excellent stability with 99% initial capacitance retention after 1000 charge/discharge cycles. GH/PANI composites synthesized at 0 °C and 25 °C therefore hold promise for use in supercapacitor device applications.

Novel concept of the smart NIR-light-controlled drug release of black phosphorus nanostructure for cancer therapy.

PubMed

Qiu, Meng; Wang, Dou; Liang, Weiyuan; Liu, Liping; Zhang, Yin; Chen, Xing; Sang, David Kipkemoi; Xing, Chenyang; Li, Zhongjun; Dong, Biqin; Xing, Feng; Fan, Dianyuan; Bao, Shiyun; Zhang, Han; Cao, Yihai

2018-01-16

A biodegradable drug delivery system (DDS) is one the most promising therapeutic strategies for cancer therapy. Here, we propose a unique concept of light activation of black phosphorus (BP) at hydrogel nanostructures for cancer therapy. A photosensitizer converts light into heat that softens and melts drug-loaded hydrogel-based nanostructures. Drug release rates can be accurately controlled by light intensity, exposure duration, BP concentration, and hydrogel composition. Owing to sufficiently deep penetration of near-infrared (NIR) light through tissues, our BP-based system shows high therapeutic efficacy for treatment of s.c. cancers. Importantly, our drug delivery system is completely harmless and degradable in vivo. Together, our work proposes a unique concept for precision cancer therapy by external light excitation to release cancer drugs. If these findings are successfully translated into the clinic, millions of patients with cancer will benefit from our work.

Supramolecular Amino Acid Based Hydrogels: Probing the Contribution of Additive Molecules using NMR Spectroscopy

PubMed Central

Ramalhete, Susana M.; Nartowski, Karol P.; Sarathchandra, Nichola; Foster, Jamie S.; Round, Andrew N.; Angulo, Jesús

2017-01-01

Abstract Supramolecular hydrogels are composed of self‐assembled solid networks that restrict the flow of water. l‐Phenylalanine is the smallest molecule reported to date to form gel networks in water, and it is of particular interest due to its crystalline gel state. Single and multi‐component hydrogels of l‐phenylalanine are used herein as model materials to develop an NMR‐based analytical approach to gain insight into the mechanisms of supramolecular gelation. Structure and composition of the gel fibres were probed using PXRD, solid‐state NMR experiments and microscopic techniques. Solution‐state NMR studies probed the properties of free gelator molecules in an equilibrium with bound molecules. The dynamics of exchange at the gel/solution interfaces was investigated further using high‐resolution magic angle spinning (HR‐MAS) and saturation transfer difference (STD) NMR experiments. This approach allowed the identification of which additive molecules contributed in modifying the material properties. PMID:28401991

Interaction of Human Plasma Proteins with Thin Gelatin-Based Hydrogel Films: A QCM-D and ToF-SIMS Study

PubMed Central

2015-01-01

In the fields of surgery and regenerative medicine, it is crucial to understand the interactions of proteins with the biomaterials used as implants. Protein adsorption directly influences cell-material interactions in vivo and, as a result, regulates, for example, cell adhesion on the surface of the implant. Therefore, the development of suitable analytical techniques together with well-defined model systems allowing for the detection, characterization, and quantification of protein adsorbates is essential. In this study, a protocol for the deposition of highly stable, thin gelatin-based films on various substrates has been developed. The hydrogel films were characterized morphologically and chemically. Due to the obtained low thickness of the hydrogel layer, this setup allowed for a quantitative study on the interaction of human proteins (albumin and fibrinogen) with the hydrogel by Quartz Crystal Microbalance with Dissipation Monitoring (QCM-D). This technique enables the determination of adsorbant mass and changes in the shear modulus of the hydrogel layer upon adsorption of human proteins. Furthermore, Secondary Ion Mass Spectrometry and principal component analysis was applied to monitor the changed composition of the topmost adsorbate layer. This approach opens interesting perspectives for a sensitive screening of viscoelastic biomaterials that could be used for regenerative medicine. PMID:24956040

Superporous hybrid hydrogels based on polyacrylamide and chitosan: Characterization and in vitro drug release

PubMed Central

Nagpal, Manju; Singh, Shailendra Kumar; Mishra, Dinanath

2013-01-01

Objective: Current research was aimed at the development of the drug delivery systems based on the superporous hydrogels (SPH) with the desired swelling and the mechanical properties. Materials and Methods: Superporous hydrogel composites (SPHCs) and superporous hybrid hydrogels (SPHHs) based on the chitosan and the polyacrylamide were synthesized using the gas blowing technique. The prepared hydrogels were evaluated for swelling studies, mechanical strength and scanning electron microscopy. The selected hydrogels were loaded with the drug (verapamil hydrochloride) by aqueous loading method. Drug integrity with in polymeric network was evaluated via fourier transform infrared spectroscopy (FTIR), X-ray diffraction (X-RD), differential scanning calorimetry (DSC), proton nuclear magnetic resonance (1HNMR) studies. In vitro drug release studies were carried out using the united state pharmacopoeial (USP) dissolution apparatus (type II). Results and Discussion: The mechanical strength was observed to be higher in SPH hybrids in comparison to that in SPHCs while no significant difference was observed in swelling behavior. In situ crosslinking of chitosan with glutaraldehyde (GA) may be responsible for high mechanical strength. The equilibrium swelling time was slight higher in SPHH than in SPHCs. The integrity of pores was maintained in ethanol treated hydrogels as observed in scanning electron micrographs. Whereas, freeze dried SPH samples showed non-uniform pores. No drug polymer interaction was observed as indicated by DSC, FTIR, X-RD and NMR studies. However, the crosslinking of chitosan with GA was clearly indicated by these studies. The in vitro drug release studies from SPH hybrids indicated initial fast release (65%) with in first 2 h and then sustained release at the end of 24 h (95%). The addition of hydroxypropyl methyl cellulose with drug; however, leads to a significant decrease in drug release (56% at the end of 24 h). Conclusion: Superporous hybrid hydrogels can be promising devices for the sustained delivery of drug candidates to the gastrointestinal region. PMID:24015380

Degradable Bone Graft Substitute for Effective Delivery of Multiple Growth Factors in the Treatment of Nonunion Fractures

DTIC Science & Technology

2011-10-01

During this reporting period, a more general set of hydrogel synthesis steps were defined which enables the incorporation of chitosan from multiple...sources and suppliers and still produce a consistent material. Functional behavior of the hydrogel was confirmed with a new source of chitosan ...inducing tissue ingrowth into a subcutaneously injected scaffold loaded with the composite xylan/ chitosan hydrogel. Delivery of new hydrogel treatment for

Comparison of H2S adsorption by two hydrogel composite (HBC) derived by Empty Fruit Bunch (EFB) biochar and Coal Fly Ash (CFA)

NASA Astrophysics Data System (ADS)

Meri, N. H.; Alias, A. B.; Talib, N.; Rashid, Z. A.; Ghani, W. A. W. A. K.

2018-03-01

This study are covered the adsorption performance of two adsorbent Empty Fruit Bunch Hydrogel Biochar Composite (EFB-HBC) and Coal Fly Ash Hydrogel Composite (CFA-HC) on hydrogen sulphide. The EFB biochar were produce by pyrolysed and heated from room temperature to 550˚C at 10˚C/min under the Nitrogen flow. Meanwhile, coal fly ash collected from a power plant located in Selangor, Malaysia. Both of the materials is a waste from different industries and became the precursor to our adsorbents. EFB biochar and coal fly ash has been synthesized to become hydrogel by polymerization process with acrylamide (AAm) as monomer, N,N’-methylene bisacry lamide (MBA) as cross linker and ammonium persulfate (APS) as initiator. In addition, because of the speciality of hydrogel itself, which is has high ability in storing water, the effect of H2O wetness on EFB-HBC and CFA-HC were investigate in adsorption of H2S. EFB-HBC gave a longest breakthrough time and highest adsorption capacity compared with CFA-HC in both condition (dry/wet). The result also indicated that, the increased the bed height, increased the adsorption capacity.

Thermo-responsive and compression properties of TEMPO-oxidized cellulose nanofiber-modified PNIPAm hydrogels.

PubMed

Wei, Jinguang; Chen, Yufei; Liu, Hongzhi; Du, Chungui; Yu, Huilong; Zhou, Zhongxi

2016-08-20

In this study, TEMPO-oxidized bamboo cellulose nanofibers (TO-CNF) with anionic carboxylate groups on the surfaces were in-situ incorporated into poly(N-isopropylacrylamide) (PNIPAm) matrix to improve its thermo-responsive and mechanical properties during the polymerization. The microstructure, swelling behaviors, and compressive strength of resultant PNIPAm composite hydrogels with varying contents of TO-CNFs (0-10wt%) were then examined, respectively. Modified hydrogels exhibited the similar light transparency to pure PNIPAm one due to the formation of semi-IPN structure between PNIPAm and TO-CNF. FT-IR spectra demonstrated that the presence of TO-CNF did not alter the position of characteristic peaks associated with PNIPAm. SEM observation suggested that the pore size of PNIPAm hydrogels was markedly increased after the incorporation of TO-CNF. Also, the composite hydrogels showed superior swelling behavior and much improved compression properties with respect to pure PNIPAm one. Thus, TO-CNF appeared to be a "green" nanofiller that can simultaneously improve swelling and mechanical properties of PNIPAm hydrogel. Copyright © 2016 Elsevier Ltd. All rights reserved.

Hyaluronic acid based hydrogel system for soft tissue regeneration and drug delivery

NASA Astrophysics Data System (ADS)

Jha, Amit Kumar

We have developed hyaluronic acid (HA)-based, biomimetic hydrogel matrices that are hierarchically structured, mechanically robust and biologically active. Specifically, HA-based hydrogel particles (HGPs) with controlled sizes, defined porosity, and improved stability were synthesized using different inverse emulsion systems and crosslinking chemistries. The resultant particles either contained residual functional groups or were rendered reactive by subsequent chemical modifications. HA-based doubly crosslinked networks (DXNs) were synthesized via covalent crosslinking of HA HGPs with soluble HA macromers carrying mutually reactive functional groups. These hybrid matrices are hierarchical in nature, consisting of densely crosslinked HGPs integrated in a loosely connected secondary matrix. Their mechanical properties and degradation kinetics can be readily tuned by varying the particle size, functional group density, intra- and interparticle crosslinking. To improve the biological functions of HA HGPs, perlecan domain I (PlnDI), a basement membrane proteoglycan that has strong affinity for various heparin binding growth factors (HBGFs), was successfully conjugated to the particles through the core protein via a flexible poly(ethylene glycol) (PEG) linker. The immobilized PlnDI maintains its ability to bind bone morphogenetic proteins (BMP-2) and modulates its in vitro release. A similar, sustained release of BMP-2 was achieved by encapsulating BMP-2-loaded HGPs within a photocrosslinked HA matrix. When encapsulated in HA DXNs, primary bovine chondrocytes were able to maintain their phenotype, proliferate readily and produce abundant glycosaminoglycan. Finally, cell-adhesive HA DXNs were fabricated by encapsulating gelatin-decorated HA HGPs in a secondary HA matrix. Human MSCs were shown to adhere to the composite matrix through the focal adhesion sites clustered on particle surface. The cell-adhesive composite matrices supported hMSC proliferation and migration into the gels. Human MSCs were undifferentiated during the early time points of culture, however differentiated into osteoblast phenotype after 28 days of culture. In summary, the HA-based hydrogel matrices are hierarchically structured, mechanically robust and enzymatically stable, capable of mediating cellular functions through the spatial and temporal presentation of defined biological cues. These hydrogel systems are promising candidates for soft tissue regeneration.

Two-Step Self-Assembly of Liposome-Multidomain Peptide Nanofiber Hydrogel for Time-Controlled Release

PubMed Central

2015-01-01

Progress in self-assembly and supramolecular chemistry has been directed toward obtaining macromolecular assemblies with higher degrees of complexity, simulating the highly structured environment in natural systems. One approach to this type of complexity are multistep, multicomponent, self-assembling systems that allow approaches comparable to traditional multistep synthetic organic chemistry; however, only a few examples of this approach have appeared in the literature. Our previous work demonstrated nanofibrous mimics of the extracellular matrix. Here we demonstrate the ability to create a unique hydrogel, developed by stepwise self-assembly of multidomain peptide fibers and liposomes. The two-component system allows for controlled release of bioactive factors at multiple time points. The individual components of the self-assembled gel and the composite hydrogel were characterized by TEM, SEM, and rheometry, demonstrating that peptide nanofibers and lipid vesicles both retain their structural integrity in the composite gel. The rheological robustness of the hydrogel is shown to be largely unaffected by the presence of liposomes. Release studies from the composite gels loaded with different growth factors EGF, MCP-1, and PlGF-1 showed delay and prolongation of release by liposomes entrapped in the hydrogel compared to more rapid release from the hydrogel alone. This bimodal release system may have utility in systems where timed cascades of biological signals may be valuable, such as in tissue regeneration. PMID:25308335

A Review of the Development of a Vehicle for Localized and Controlled Drug Delivery for Implantable Biosensors

PubMed Central

Bhardwaj, Upkar; Papadimitrakopoulos, Fotios; Burgess, Diane J.

2008-01-01

A major obstacle to the development of implantable biosensors is the foreign body response (FBR) that results from tissue trauma during implantation and the continuous presence of the implant in the body. The in vivo stability and functionality of biosensors are compromised by damage to sensor components and decreased analyte transport to the sensor. This paper summarizes research undertaken by our group since 2001 to control the FBR toward implanted sensors. Localized and sustained delivery of the anti-inflammatory drug, dexamethasone, and the angiogenic growth factor, vascular endothelial growth factor (VEGF), was utilized to inhibit inflammation as well as fibrosis and provide a stable tissue–device interface without producing systemic adverse effects. The drug-loaded polylactic-co-glycolic acid (PLGA) microspheres were embedded in a polyvinyl alcohol (PVA) hydrogel composite to fabricate a drug-eluting, permeable external coating for implantable devices. The composites were fabricated using the freeze–thaw cycle method and had mechanical properties similar to soft body tissue. Dexamethasone-loaded microsphere/hydrogel composites were able to provide anti-inflammatory protection, preventing the FBR. Moreover, concurrent release of dexamethasone with VEGF induced neoangiogenesis in addition to providing anti-inflammatory protection. Sustained release of dexamethasone is required for the entire sensor lifetime, as a delayed inflammatory response developed after depletion of the drug from the composites. These studies have shown the potential of PLGA microsphere/PVA hydrogel-based composites as drug-eluting external coatings for implantable biosensors. PMID:19885291

Emerging Technologies for Assembly of Microscale Hydrogels

PubMed Central

Kavaz, Doga; Demirel, Melik C.; Demirci, Utkan

2013-01-01

Assembly of cell encapsulating building blocks (i.e., microscale hydrogels) has significant applications in areas including regenerative medicine, tissue engineering, and cell-based in vitro assays for pharmaceutical research and drug discovery. Inspired by the repeating functional units observed in native tissues and biological systems (e.g., the lobule in liver, the nephron in kidney), assembly technologies aim to generate complex tissue structures by organizing microscale building blocks. Novel assembly technologies enable fabrication of engineered tissue constructs with controlled properties including tunable microarchitectural and predefined compositional features. Recent advances in micro- and nano-scale technologies have enabled engineering of microgel based three dimensional (3D) constructs. There is a need for high-throughput and scalable methods to assemble microscale units with a complex 3D micro-architecture. Emerging assembly methods include novel technologies based on microfluidics, acoustic and magnetic fields, nanotextured surfaces, and surface tension. In this review, we survey emerging microscale hydrogel assembly methods offering rapid, scalable microgel assembly in 3D, and provide future perspectives and discuss potential applications. PMID:23184717

Ultrasonic characterization of silicate glasses, polymer composites and hydrogels

NASA Astrophysics Data System (ADS)

Lee, Wan Jae

In many applications of material designing and engineering, high-frequency linear viscoelastic properties of materials are essential. Traditionally, the high-frequency properties are estimated through the time-temperature superposition (WLF equation) of low-frequency data, which are questionable because the existence of multi-phase in elastomer compounds. Moreover, no reliable data at high frequencies over MHz have been available thus far. Ultrasound testing is cost-effective for measuring high-frequency properties. Although both ultrasonic longitudinal and shear properties are necessary in order to fully characterize high-frequency mechanical properties of materials, longitudinal properties will be extensively explored in this thesis. Ultrasonic pulse echo method measures longitudinal properties. A precision ultrasonic measurement system has been developed in our laboratory, which allows us to monitor the in-situ bulk and/or surface properties of silicate glasses, polymer composites and even hydrogels. The system consists of a pulse-echo unit and an impedance measurement unit. A pulse echo unit is explored mainly. First, a systematic procedure was developed to obtain precise water wavespeed value. A calibration curve of water wavespeed as a function of temperature has been established, and water wavespeed at 23°C serves as a yardstick to tell whether or not a setup is properly aligned. Second, a sound protocol in calculating attenuation coefficient and beam divergence effects was explored using three kinds of silicate glass of different thicknesses. Then the system was applied to four composite slabs, two slabs for each type of fiberglass reinforced plastics, phenolic and polyester manufactured under different processing conditions: one was made by the normal procedures and the other with deliberate flaws such as voids, tapes and/or prepared at improper operation temperature and pressure. The experiment was conducted under the double blind test protocol. After carefully and methodically analyzing the data, we are able to detect defected specimens from all the specimens supplied to us, differentiate polyester-based composite from the phenolic-based composite and even recognized types of defects. Lastly, ultrasonic monitoring of advancement of the swollen-unswollen fronts, and hence monitor phase transition from glassy state to rubbery state, of poly(acrylic-acid) hydrogel of one of the three different crosslinking densities is performed. With ultrasonic measurement, swelling monitoring is possible since the structural and mechanical changes during swelling of a dry hydrogel are related to changes in density and elastic constants. Using our carefully developed methodology from previous chapters, we may obtain and monitor average acoustic properties of each layer of hydrogel as it swells.

A Bioinspired Alginate-Gum Arabic Hydrogel with Micro-/Nanoscale Structures for Controlled Drug Release in Chronic Wound Healing.

PubMed

Li, Mi; Li, Haichang; Li, Xiangguang; Zhu, Hua; Xu, Zihui; Liu, Lianqing; Ma, Jianjie; Zhang, Mingjun

2017-07-12

Biopolymeric hydrogels have drawn increasing research interest in biomaterials due to their tunable physical and chemical properties for both creating bioactive cellular microenvironment and serving as sustainable therapeutic reagents. Inspired by a naturally occurring hydrogel secreted from the carnivorous Sundew plant for trapping insects, here we have developed a bioinspired hydrogel to deliver mitsugumin 53 (MG53), an important protein in cell membrane repair, for chronic wound healing. Both chemical compositions and micro-/nanomorphological properties inherent from the natural Sundew hydrogel were mimicked using sodium alginate and gum arabic with calcium ion-mediated cross-linking. On the basis of atomic force microscopy (AFM) force measurements, an optimal sticky hydrogel scaffold was obtained through orthogonal experimental design. Imaging and mechanical analysis showed the distinct correlation between structural morphology, adhesion characteristics, and mechanical properties of the Sundew-inspired hydrogel. Combined characterization and biochemistry techniques were utilized to uncover the underlying molecular composition involved in the interactions between hydrogel and protein. In vitro drug release experiments confirmed that the Sundew-inspired hydrogel had a biphasic-kinetics release, which can facilitate both fast delivery of MG53 for improving the reepithelization process of the wounds and sustained release of the protein for treating chronic wounds. In vivo experiments showed that the Sundew-inspired hydrogel encapsulating with rhMG53 could facilitate dermal wound healing in mouse model. Together, these studies confirmed that the Sundew-inspired hydrogel has both tunable micro-/nanostructures and physicochemical properties, which enable it as a delivery vehicle for chronic wounding healing. The research may provide a new way to develop biocompatible and tunable biomaterials for sustainable drug release to meet the needs of biological activities.

Extracellular Matrix Hydrogel Derived from Human Umbilical Cord as a Scaffold for Neural Tissue Repair and Its Comparison with Extracellular Matrix from Porcine Tissues.

PubMed

Kočí, Zuzana; Výborný, Karel; Dubišová, Jana; Vacková, Irena; Jäger, Aleš; Lunov, Oleg; Jiráková, Klára; Kubinová, Šárka

2017-06-01

Extracellular matrix (ECM) hydrogels prepared by tissue decellularization have been reported as natural injectable materials suitable for neural tissue repair. In this study, we prepared ECM hydrogel derived from human umbilical cord (UC) and evaluated its composition and mechanical and biological properties in comparison with the previously described ECM hydrogels derived from porcine urinary bladder (UB), brain, and spinal cord. The ECM hydrogels did not differ from each other in the concentration of collagen, while the highest content of glycosaminoglycans as well as the shortest gelation time was found for UC-ECM. The elastic modulus was then found to be the highest for UB-ECM. In spite of a different origin, topography, and composition, all ECM hydrogels similarly promoted the migration of human mesenchymal stem cells (MSCs) and differentiation of neural stem cells, as well as axonal outgrowth in vitro. However, only UC-ECM significantly improved proliferation of tissue-specific UC-derived MSCs when compared with the other ECMs. Injection of UC-ECM hydrogels into a photothrombotic cortical ischemic lesion in rats proved its in vivo gelation and infiltration with host macrophages. In summary, this study proposes UC-ECM hydrogel as an easily accessible biomaterial of human origin, which has the potential for neural as well as other soft tissue reconstruction.

Bioprinting 3D cell-laden hydrogel microarray for screening human periodontal ligament stem cell response to extracellular matrix.

PubMed

Ma, Yufei; Ji, Yuan; Huang, Guoyou; Ling, Kai; Zhang, Xiaohui; Xu, Feng

2015-12-22

Periodontitis is an inflammatory disease negatively affecting up to 15% of adults worldwide. Periodontal ligament stem cells (PDLSCs) hold great promises for periodontal tissue regeneration, where it is necessary to find proper extracellular matrix (ECM) materials (e.g., composition, concentration). In this study, we proposed a bioprinting-based approach to generate nano-liter sized three-dimensional (3D) cell-laden hydrogel array with gradient of ECM components, through controlling the volume ratio of two hydrogels, such as gelatin methacrylate (GelMA) and poly(ethylene glycol) (PEG) dimethacrylate. The resulting cell-laden array with a gradient of GelMA/PEG composition was used to screen human PDLSC response to ECM. The behavior (e.g., cell viability, spreading) of human PDLSCs in GelMA/PEG array were found to be depended on the volume ratios of GelMA/PEG, with cell viability and spreading area decreased along with increasing the ratio of PEG. The developed approach would be useful for screening cell-biomaterial interaction in 3D and promoting regeneration of functional tissue.

Rheological Properties of Cross-Linked Hyaluronan–Gelatin Hydrogels for Tissue Engineering

PubMed Central

Vanderhooft, Janssen L.; Alcoutlabi, Mataz; Magda, Jules J.; Prestwich, Glenn D.

2009-01-01

Hydrogels that mimic the natural extracellular matrix (ECM) are used in three-dimensional cell culture, cell therapy, and tissue engineering. A semi-synthetic ECM based on cross-linked hyaluronana offers experimental control of both composition and gel stiffness. The mechanical properties of the ECM in part determine the ultimate cell phenotype. We now describe a rheological study of synthetic ECM hydrogels with storage shear moduli that span three orders of magnitude, from 11 to 3 500 Pa, a range important for engineering of soft tissues. The concentration of the chemically modified HA and the cross-linking density were the main determinants of gel stiffness. Increase in the ratio of thiol-modified gelatin reduced gel stiffness by diluting the effective concentration of the HA component. PMID:18839402

Hydrogels Derived from Central Nervous System Extracellular Matrix

PubMed Central

Medberry, Christopher J.; Crapo, Peter M.; Siu, Bernard F.; Carruthers, Christopher A.; Wolf, Matthew T.; Nagarkar, Shailesh P.; Agrawal, Vineet; Jones, Kristen E.; Kelly, Jeremy; Johnson, Scott A.; Velankar, Sachin S.; Watkins, Simon C.; Modo, Michel

2012-01-01

Biologic scaffolds composed of extracellular matrix (ECM) are commonly used repair devices in preclinical and clinical settings; however the use of these scaffolds for peripheral and central nervous system (CNS) repair has been limited. Biologic scaffolds developed from brain and spinal cord tissue have recently been described, yet the conformation of the harvested ECM limits therapeutic utility. An injectable CNS-ECM derived hydrogel capable of in vivo polymerization and conformation to irregular lesion geometries may aid in tissue reconstruction efforts following complex neurologic trauma. The objectives of the present study were to develop hydrogel forms of brain and spinal cord ECM and compare the resulting biochemical composition, mechanical properties, and neurotrophic potential of a brain derived cell line to a non-CNS-ECM hydrogel, urinary bladder matrix. Results showed distinct differences between compositions of brain ECM, spinal cord ECM, and urinary bladder matrix. The rheologic modulus of spinal cord ECM hydrogel was greater than that of brain ECM and urinary bladder matrix. All ECMs increased the number of cells expressing neurites, but only brain ECM increased neurite length, suggesting a possible tissue-specific effect. All hydrogels promoted three-dimensional uni- or bi-polar neurite outgrowth following 7 days in culture. These results suggest that CNS-ECM hydrogels may provide supportive scaffolding to promote in vivo axonal repair. PMID:23158935

30 s Response Time of K+ Ion-Selective Hydrogels Functionalized with 18-Crown-6 Ether Based on QCM Sensor.

PubMed

Zhang, Zhenxiao; Dou, Qian; Gao, Hongkai; Bai, Bing; Zhang, Yongmei; Hu, Debo; Yetisen, Ali K; Butt, Haider; Yang, Xiaoxia; Li, Congju; Dai, Qing

2018-03-01

Potassium detection is critical in monitoring imbalances in electrolytes and physiological status. The development of rapid and robust potassium sensors is desirable in clinical chemistry and point-of-care applications. In this study, composite supramolecular hydrogels are investigated: polyethylene glycol methacrylate and acrylamide copolymer (P(PEGMA-co-AM)) are functionalized with 18-crown-6 ether by employing surface initiated polymerization. Real-time potassium ion monitoring is realized by combining these compounds with quartz crystal microbalance. The device demonstrates a rapid response time of ≈30 s and a concentration detection range from 0.5 to 7.0 × 10 -3 m. These hydrogels also exhibit high reusability and K + ion selectivity relative to other cations in biofluids such as Na + , NH 4 + , Mg 2+ , and Ca 2+ . These results provide a new approach for sensing alkali metal ions using P(PEGMA-co-AM) hydrogels. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Micro- and nano-hydroxyapatite as active reinforcement for soft biocomposites.

PubMed

Munarin, F; Petrini, P; Gentilini, R; Pillai, R S; Dirè, S; Tanzi, M C; Sglavo, V M

2015-01-01

Pectin-based biocomposite hydrogels were produced by internal gelation, using different hydroxyapatite (HA) powders from commercial source or synthesized by the wet chemical method. HA possesses the double functionality of cross-linking agent and inorganic reinforcement. The mineralogical composition, grain size, specific surface area and microstructure of the hydroxyapatite powders are shown to strongly influence the properties of the biocomposites. Specifically, the grain size and specific surface area of the HA powders are strictly correlated to the gelling time and rheological properties of the hydrogels at room temperature. Pectin pH is also significant for the formation of ionic cross-links and therefore for the hydrogels stability at higher temperatures. The obtained results point out that micrometric-size hydroxyapatite can be proposed for applications which require rapid gelling kinetics and improved mechanical properties; conversely the nanometric hydroxyapatite synthesized in the present work seems the best choice to obtain homogeneous hydrogels with more easily controlled gelling kinetics. Copyright © 2014 Elsevier B.V. All rights reserved.

An injectable particle-hydrogel hybrid system for glucose-regulatory insulin delivery.

PubMed

Zhao, Fuli; Wu, Di; Yao, Dan; Guo, Ruiwei; Wang, Weiwei; Dong, Anjie; Kong, Deling; Zhang, Jianhua

2017-12-01

Long-term and daily subcutaneous injections of insulin for the treatment of insulin-dependent diabetic patients often lead to poor patient compliance and undesired complications. Phenylboronic acid (PBA)-based polymeric hydrogels have been widely considered as one of the most promising insulin delivery system to replace the frequent insulin injections. However, their applications are limited by clinically irrelevant glucose-responsive range, slow response rate, low tissue-adhesiveness and poor biodegradability, undesirable leakage at normoglycemic state. Herein, we report a novel implantable insulin hydrogel for glucose-regulated delivery of insulin based on a unique particle-hydrogel hybrid platform featuring fast glucose responsiveness at physiological pH, shear-thinning behavior for injection, tissue-adhesive function for long-lasting adherence, and full biodegradability for safe use. The system was thoroughly characterized both in vitro and in vivo and was demonstrated to hold these unique functions. Using streptozotocin-induced diabetic mice as a model, it was shown that a single subcutaneous injection of the insulin-loaded particle-hydrogel formulation led to quasi-steady-state blood glucose levels within the normal range for about two weeks. In addition, the preparation of the formulation only involved simple mixing and self-assembling processes, and thus it had great scalability and reproducibility for practical use. The highly feasible preparation, excellent performance, inherent biocompatibility and biodegradability make this novel composite hydrogel promising platform for diabetes therapy. Phenylboronic acid (PBA)-based polymeric hydrogels have been widely considered as one of the most promising insulin delivery system to replace the frequent insulin injections. However, these hydrogels, mostly based on a variety of PBA-containing acrylamide monomers, are still far from clinical reality. Building upon a unique particle-hydrogel hybrid platform, herein we report a novel implantable insulin storage and delivery system with multifunctionalities including fast glucose-sensitiveness at physiological pH, shear-thinning behavior for injection, tissue-adhesive function for long-lasting adherence, biodegradable materials for safe use and well-controlled insulin release. These unique functions were demonstrated through research both in vitro and in vivo. In addition, the preparation of the formulation was simple, and thus it had great scalability and reproducibility for practical use. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Three-dimensional bioprinting of rat embryonic neural cells.

PubMed

Lee, Wonhye; Pinckney, Jason; Lee, Vivian; Lee, Jong-Hwan; Fischer, Krisztina; Polio, Samuel; Park, Je-Kyun; Yoo, Seung-Schik

2009-05-27

We present a direct cell printing technique to pattern neural cells in a three-dimensional (3D) multilayered collagen gel. A layer of collagen precursor was printed to provide a scaffold for the cells, and the rat embryonic neurons and astrocytes were subsequently printed on the layer. A solution of sodium bicarbonate was applied to the cell containing collagen layer as nebulized aerosols, which allowed the gelation of the collagen. This process was repeated layer-by-layer to construct the 3D cell-hydrogel composites. Upon characterizing the relationship between printing resolutions and the growth of printed neural cells, single/multiple layers of neural cell-hydrogel composites were constructed and cultured. The on-demand capability to print neural cells in a multilayered hydrogel scaffold offers flexibility in generating artificial 3D neural tissue composites.

Hydrogel scaffolds for tissue engineering: Progress and challenges

PubMed Central

El-Sherbiny, Ibrahim M.; Yacoub, Magdi H.

2013-01-01

Designing of biologically active scaffolds with optimal characteristics is one of the key factors for successful tissue engineering. Recently, hydrogels have received a considerable interest as leading candidates for engineered tissue scaffolds due to their unique compositional and structural similarities to the natural extracellular matrix, in addition to their desirable framework for cellular proliferation and survival. More recently, the ability to control the shape, porosity, surface morphology, and size of hydrogel scaffolds has created new opportunities to overcome various challenges in tissue engineering such as vascularization, tissue architecture and simultaneous seeding of multiple cells. This review provides an overview of the different types of hydrogels, the approaches that can be used to fabricate hydrogel matrices with specific features and the recent applications of hydrogels in tissue engineering. Special attention was given to the various design considerations for an efficient hydrogel scaffold in tissue engineering. Also, the challenges associated with the use of hydrogel scaffolds were described. PMID:24689032

Composites of Polymer Hydrogels and Nanoparticulate Systems for Biomedical and Pharmaceutical Applications

PubMed Central

Zhao, Fuli; Yao, Dan; Guo, Ruiwei; Deng, Liandong; Dong, Anjie; Zhang, Jianhua

2015-01-01

Due to their unique structures and properties, three-dimensional hydrogels and nanostructured particles have been widely studied and shown a very high potential for medical, therapeutic and diagnostic applications. However, hydrogels and nanoparticulate systems have respective disadvantages that limit their widespread applications. Recently, the incorporation of nanostructured fillers into hydrogels has been developed as an innovative means for the creation of novel materials with diverse functionality in order to meet new challenges. In this review, the fundamentals of hydrogels and nanoparticles (NPs) were briefly discussed, and then we comprehensively summarized recent advances in the design, synthesis, functionalization and application of nanocomposite hydrogels with enhanced mechanical, biological and physicochemical properties. Moreover, the current challenges and future opportunities for the use of these promising materials in the biomedical sector, especially the nanocomposite hydrogels produced from hydrogels and polymeric NPs, are discussed. PMID:28347111

Gradient Material Strategies for Hydrogel Optimization in Tissue Engineering Applications

PubMed Central

2018-01-01

Although a number of combinatorial/high-throughput approaches have been developed for biomaterial hydrogel optimization, a gradient sample approach is particularly well suited to identify hydrogel property thresholds that alter cellular behavior in response to interacting with the hydrogel due to reduced variation in material preparation and the ability to screen biological response over a range instead of discrete samples each containing only one condition. This review highlights recent work on cell–hydrogel interactions using a gradient material sample approach. Fabrication strategies for composition, material and mechanical property, and bioactive signaling gradient hydrogels that can be used to examine cell–hydrogel interactions will be discussed. The effects of gradients in hydrogel samples on cellular adhesion, migration, proliferation, and differentiation will then be examined, providing an assessment of the current state of the field and the potential of wider use of the gradient sample approach to accelerate our understanding of matrices on cellular behavior. PMID:29485612

Applications of hydrogels in the nursery and during outplanting

Treesearch

Thomas D. Landis; Diane L. Haase

2012-01-01

Hydrogels have a variety of potential uses including application to plants in the nursery and at the time of outplanting. Absorptive capacity of these gels is influenced by their chemical and physical composition as well as the ion concentration of the liquid being absorbed. The most common uses for hydrogels in nurseries or during outplanting are incorporation or root...

In vivo results of hydrogel composite pericardial substitutes.

PubMed

Blue, M A; Guilbeau, E J; Brandon, T A; Walker, A S; Bjotvedt, G; Fisk, R L

1991-01-01

In this study, two improved pericardial patches were developed and evaluated for their efficacy as pericardial substitutes. The patches are composites consisting of a hydrogel (PHEMA) that coats an underlying mesh (either ETFE or PET). Studies were conducted using subcutaneous implants in rats and pericardial patch implants in greyhound dogs. Adhesions between the substitute and pericardium and the epicardium were minimal. The ETFE composite patch caused an unacceptable epicardial reaction. The PET patch results were encouraging; the epicardium was largely unaffected by the patch.

Enzymatic mineralization generates ultrastiff and tough hydrogels with tunable mechanics

NASA Astrophysics Data System (ADS)

Rauner, Nicolas; Meuris, Monika; Zoric, Mirjana; Tiller, Joerg C.

2017-03-01

The cartilage and skin of animals, which are made up of more than fifty per cent water, are rather stiff (having elastic moduli of up to 100 megapascals) as well as tough and hard to break (with fracture energies of up to 9,000 joules per square metre). Such features make these biological materials mechanically superior to existing synthetic hydrogels. Lately, progress has been made in synthesizing tough hydrogels, with double-network hydrogels achieving the toughness of skin and inorganic-organic composites showing even better performance. However, these materials owe their toughness to high stretchability; in terms of stiffness, synthetic hydrogels cannot compete with their natural counterparts, with the best examples having elastic moduli of just 10 megapascals or less. Previously, we described the enzyme-induced precipitation and crystallization of hydrogels containing calcium carbonate, but the resulting materials were brittle. Here we report the enzyme-induced formation of amorphous calcium phosphate nanostructures that are homogenously distributed within polymer hydrogels. Our best materials have fracture energies of 1,300 joules per square metre even in their fully water-swollen state—a value superior to that of most known water-swollen synthetic materials. We are also able to modulate their stiffness up to 440 megapascals, well beyond that of cartilage and skin. Furthermore, the highly filled composite materials can be designed to be optically transparent and to retain most of their stretchability even when notched. We show that percolation drives the mechanical properties, particularly the high stiffness, of our uniformly mineralized hydrogels.

Aromatic organic contaminant removal from an aqueous environment by p(4-VP)-based materials.

PubMed

Sahiner, Nurettin; Ozay, Ozgur; Aktas, Nahit

2011-10-01

p(4-vinylpyridine) (p(4-VP)) hydrogels were prepared in bulk (macro, 5 × 6 mm) and in nanosizes (370 nm) dimensions. The prepared hydrogels were used to remove organic aromatic contaminates such as 4-nitrophenol (4-NP), 2-nitrophenol (2-NP), phenol (Ph) and nitrobenzene (NB) from an aqueous environment. Important parameters affecting the absorption phenomena, such as the initial concentration of the organic species and the absorbent, absorption rate, absorption capacity, pH and the temperature of the medium, were evaluated for both hydrogel sizes. The absorption capacity of bulk and microgels were found to be 4-NP>2-NP>Ph>NB. Furthermore, p(4-VP) microgels were embedded in poly(acrylamide) (p(AAm)) bulk hydrogel as a microgel-hydrogel interpenetrating polymer network and proved to be very practical in overcoming the difficulty of using the microgels in real applications. Moreover, it was demonstrated that separately prepared magnetic ferrite particles inserted inside p(4-VP) microgels during synthesis allowed for trouble-free removal of p(4-VP)-magnetic composite microgels from the aqueous environment by an externally applied magnetic field upon completion of their task. Copyright © 2011 Elsevier Ltd. All rights reserved.

Photothermal-modulated drug delivery and magnetic relaxation based on collagen/poly(γ-glutamic acid) hydrogel.

PubMed

Cho, Sun-Hee; Kim, Ahreum; Shin, Woojung; Heo, Min Beom; Noh, Hyun Jong; Hong, Kwan Soo; Cho, Jee-Hyun; Lim, Yong Taik

2017-01-01

Injectable and stimuli-responsive hydrogels have attracted attention in molecular imaging and drug delivery because encapsulated diagnostic or therapeutic components in the hydrogel can be used to image or change the microenvironment of the injection site by controlling various stimuli such as enzymes, temperature, pH, and photonic energy. In this study, we developed a novel injectable and photoresponsive composite hydrogel composed of anticancer drugs, imaging contrast agents, bio-derived collagen, and multifaceted anionic polypeptide, poly (γ-glutamic acid) (γ-PGA). By the introduction of γ-PGA, the intrinsic temperature-dependent phase transition behavior of collagen was modified to a low viscous sol state at room temperature and nonflowing gel state around body temperature. The modified temperature-dependent phase transition behavior of collagen/γ-PGA hydrogels was also evaluated after loading of near-infrared (NIR) fluorophore, indocyanine green (ICG), which could transform absorbed NIR photonic energy into thermal energy. By taking advantage of the abundant carboxylate groups in γ-PGA, cationic-charged doxorubicin (Dox) and hydrophobic MnFe 2 O 4 magnetic nanoparticles were also incorporated successfully into the collagen/γ-PGA hydrogels. By illumination of NIR light on the collagen/γ-PGA/Dox/ICG/MnFe 2 O 4 hydrogels, the release kinetics of Dox and magnetic relaxation of MnFe 2 O 4 nanoparticles could be modulated. The experimental results suggest that the novel injectable and NIR-responsive collagen/γ-PGA hydrogels developed in this study can be used as a theranostic platform after loading of various molecular imaging probes and therapeutic components.

Mechanical Behavior of Tough Hydrogels for Structural Applications

NASA Astrophysics Data System (ADS)

Illeperuma, Widusha Ruwangi Kaushalya

Hydrogels are widely used in many commercial products including Jell-O, contact lenses, and superabsorbent diapers. In recent decades, hydrogels have been under intense development for biomedical applications, such as scaffolds in tissue engineering, carriers for drug delivery, and valves in microfluidic systems. But the scope is severely limited as conventional hydrogels are weak and brittle and are not very stretchable. This thesis investigates the approaches that enhance the mechanical properties of hydrogels and their structural applications. We discov¬ered a class of exceptionally stretchable and tough hydrogels made from poly-mers that form networks via ionic and covalent crosslinks. Although such a hydrogel contains ~90% water, it can be stretched beyond 20 times its initial length, and has a fracture energy of ~9000 J/m2. The combination of large stretchability, remarkable toughness, and recoverability of stiffness and toughness, along with easy synthesis makes this material much superior over existing hydrogels. Extreme stretchability and blunted crack tips of these hydrogels question the validity of traditional fracture testing methods. We re-examine a widely used pure shear test method to measure the fracture energy. With the experimental and simulation results, we conclude that the pure shear test method can be used to measure fracture energy of extremely stretchable materials. Even though polyacrylamide-alginate hydrogels have an extremely high toughness, it has a relatively low stiffness and strength. We improved the stiffness and strength by embedding fibers. Most hydrogels are brittle, allowing the fibers to cut through the hydrogel when the composite is loaded. But tough hydrogel composites do not fail by the fibers cutting the hydrogel; instead, it undergoes large deforming by fibers sliding through the matrix. Hydrogels were not considered as materials for structural applications. But with enhanced mechanical properties, they have opened up novel applications. This thesis aims to investigate the broader applications, well beyond those investigated so far. We show fiber reinforced tough hydrogels can dissipate a significant amount of energy at a tunable level of stress, making them suitable for energy absorbing applications such as inner layer of helmets. We develop inexpensive fire-retarding materials using tough hydrogels that provide superior protection from burn injuries. We also study hydrogels as actuators that can be used in soft robotics. Hydrogels contain mostly water and they freeze when the temperature drops below 00C and lose its functions. We demonstrate a new class of hydrogels that do not freeze and hydrogels that partially freeze below water freezing temperature. Partially freezing hydrogels are ideal for cooling applications such as gel packs and non-freezing hydrogels are useful in all the structural applications at low temperatures. This thesis will enable the use of inexpensive hydrogels in a new class of non-traditional structural applications where the mechanical behavior of the hydrogel is of prime importance.

Bio-inspired Self-healing Composite Hydrogel with Iron Oxide Nanoparticle as Coordination Crosslinker

NASA Astrophysics Data System (ADS)

Li, Qiaochu; Barret, Devin G.; Messersmith, Phillip B.; Holten-Andersen, Niels

2014-03-01

Polymer-nanoparticle (NP) composites have attracted renewed attention due to enhanced mechanical strength combined with various functionalities, but controlling the interfacial chemistry between NPs and polymer matrix, which is crucial for the composite's mechanical behavior, remains a major challenge. Inspired by the adhesion chemistry of mussel fibers, we investigated a novel approach to incorporate Fe3O4 NPs into hydrogel matrix. A polyethylene glycol polymer is designed with both ends conjugated by catechol groups, which have strong coordination affinity to Fe. The polymer network is crosslinked via coordination bonding at the surface of Fe3O4 NPs, yielding a stiff nanocomposite hydrogel. Due to the reversible nature of coordination bonding, the hydrogel presents self-healing behavior. Oscillatory rheology allows comparative kinetic studies of self-healing driven by catechol bonding at Fe3O4 NP interfaces and by catechol-Fe3+ coordination complexes. Furthermore, the superparamagnetic property of Fe3O4 NP is preserved after gelation, allowing for response to external stimuli. This gelation motif can serve as a versatile platform for tuning functional and mechanical properties for future polymer nanocomposite materials.

Poroelasticity-driven lubrication in hydrogel interfaces.

PubMed

Reale, Erik R; Dunn, Alison C

2017-01-04

It is widely accepted that hydrogel surfaces are slippery, and have low friction, but dynamic applied stresses alter the hydrogel composition at the interface as water is displaced. The induced osmotic imbalance of compressed hydrogel which cannot swell to equilibrium should drive the resistance to slip against it. This paper demonstrates the driving role of poroelasticity in the friction of hydrogel-glass interfaces, specifically how poroelastic relaxation of hydrogels increases adhesion. We translate the work of adhesion into an effective surface energy density that increases with the duration of applied pressure from 10 to 50 mJ m -2 , as measured by micro-indentation. A model of static friction coefficient is derived from an area-based rules of mixture for the surface energies, and predicts the friction coefficient changes upon initiation of slip. For kinetic friction, the competition between duration of contact and relaxation time is quantified by a contacting Péclet number, Pe C . A single length parameter on the scale of micrometers fits these two models to experimental micro-friction data. These models predict how short durations of applied pressure and faster sliding speeds, do not disrupt interfacial hydration; this prevailing water maintains low friction. At low speeds where interface drainage dominates, the osmotic suction works against slip for higher friction. The prediction of friction coefficients after adhesion characterization by micro-indentation makes use of the interplay between poroelasticity, adhesion, and friction. This approach provides a starting point for prediction of, and design for, hydrogel interfacial friction.

Switchable on/off drug release from gold nanoparticles-grafted dual light- and temperature-responsive hydrogel for controlled drug delivery.

PubMed

Amoli-Diva, Mitra; Sadighi-Bonabi, Rasoul; Pourghazi, Kamyar

2017-07-01

A switchable dual light- and temperature-responsive drug carrier using gold nanoparticles (Au NPs)-grafted poly(dimethylacrylamide-co-acrylamide)/poly acrylic acid [P(DMA-co-AAm)/PAAc] hydrogel was prepared by free radical polymerization procedure using N,N-methylenebisacrylamide as cross-linker and ammonium persulfate as initiator. Initial P(DMA-co-AAm) hydrogel and uniformly-distributed stable Au NPs, prepared by reduction of hydrogen tetrachloroaureate (III) hydrate in the presence of trisodium citrate, were synthesized separately. Then, the prepared P(DMA-co-AAm) and Au NPs were added to an acrylic acid solution along with the cross-linker and initiator to prepare PAAc hydrogel within the mixture. This improves the swelling ratio and stabilizes Au NPs in networks. Furthermore, a cross-linked P(DMA-co-AAm-co-AAc) random hydrogel was also prepared with the same monomer compositions as the above hydrogel for comparison of their properties. Then, swelling, thermal sensitivity and thermal and optical switching properties of the prepared hydrogels were investigated in two acidic (pH=1.2) and neutral (pH=7.4) buffered solutions to simulate stomach and intestine body conditions. Finally, loading and cumulative release (%) of ofloxacin antibiotic as model drug were considered in both thermal and optical switching conditions. Based on these results, pulsatile release vehicle was obtained which have the "on" state at higher temperatures and the "off" state at lower temperatures. Copyright © 2017 Elsevier B.V. All rights reserved.

Recent Advances in Hydrogel-Based Drug Delivery for Melanoma Cancer Therapy: A Mini Review

PubMed Central

Elupula, Ravinder

2017-01-01

The purpose of this study is to describe some of the latest advances in using hydrogels for cancer melanoma therapy. Hydrogel formulations of polymeric material from natural or synthetic sources combined with therapeutic agents have gained great attention in the recent years for treating various maladies. These formulations can be categorized according to the strategies that induce cancer cell death in melanoma. First of all, we should note that these formulations can only play a supporting role that releases bioactive agents against cancer cells rather than the main role. This strategy involves delivering the drug via transdermal pathways, resulting in the death of cancerous cells. Another strategy utilizes magnetic gel composites to combat melanoma via hyperthermia therapy. This review discusses both transdermal and hyperthermia therapies and the recent advances that have occurred in the field. PMID:28852576

A study on the effect of the concentration of N,N-methylenebisacrylamide and acrylic acid toward the properties of Dioscorea hispida-starch-based hydrogel

NASA Astrophysics Data System (ADS)

Ashri, Airul; Lazim, Azwan

2014-09-01

The research investigated the effects of acrylic acid (monomer) and N,N,-methylenebisacrylamide, MBA (crosslinker) toward the percentage of gel content, swelling ratio and ionic strength of a starch-based hydrogel. Starch grafted on poly (sodium acrylate), St-g-PAANa hydrogel was prepared by incorporating starch extracted from Dioscorea hispida in NaOH/aqueous solution using different composition of acrylic acid (AA) and N,N-methylenebisacrylamide (MBA) in the presence of potassium persulfate (KPS) as chemical initiator. The highest gel content was observed at 1:30 ratio of starch to AA and 0.10 M of MBA. Results showed the highest swelling ratio was observed at 1:15 ratio of starch to acrylic acid and 0.02 M of MBA solution. The same results also gave the highest swelling ratio for the ionic strength study. The FTIR analysis was also conducted in order to confirm the grafting of AA onto starch backbone.

A protocol for rheological characterization of hydrogels for tissue engineering strategies.

PubMed

Zuidema, Jonathan M; Rivet, Christopher J; Gilbert, Ryan J; Morrison, Faith A

2014-07-01

Hydrogels are studied extensively for many tissue engineering applications, and their mechanical properties influence both cellular and tissue compatibility. However, it is difficult to compare the mechanical properties of hydrogels between studies due to a lack of continuity between rheological protocols. This study outlines a straightforward protocol to accurately determine hydrogel equilibrium modulus and gelation time using a series of rheological tests. These protocols are applied to several hydrogel systems used within tissue engineering applications: agarose, collagen, fibrin, Matrigel™, and methylcellulose. The protocol is outlined in four steps: (1) Time sweep to determine the gelation time of the hydrogel. (2) Strain sweep to determine the linear-viscoelastic region of the hydrogel with respect to strain. (3) Frequency sweep to determine the linear equilibrium modulus plateau of the hydrogel. (4) Time sweep with values obtained from strain and frequency sweeps to accurately report the equilibrium moduli and gelation time. Finally, the rheological characterization protocol was evaluated using a composite Matrigel™-methylcellulose hydrogel blend whose mechanical properties were previously unknown. The protocol described herein provides a standardized approach for proper analysis of hydrogel rheological properties. © 2013 Wiley Periodicals, Inc.

Enhanced mechanical properties of thermosensitive chitosan hydrogel by silk fibers for cartilage tissue engineering.

PubMed

Mirahmadi, Fereshteh; Tafazzoli-Shadpour, Mohammad; Shokrgozar, Mohammad Ali; Bonakdar, Shahin

2013-12-01

Articular cartilage has limited repair capability following traumatic injuries and current methods of treatment remain inefficient. Reconstructing cartilage provides a new way for cartilage repair and natural polymers are often used as scaffold because of their biocompatibility and biofunctionality. In this study, we added degummed chopped silk fibers and electrospun silk fibers to the thermosensitive chitosan/glycerophosphate hydrogels to reinforce two hydrogel constructs which were used as scaffold for hyaline cartilage regeneration. The gelation temperature and gelation time of hydrogel were analyzed by the rheometer and vial tilting method. Mechanical characterization was measured by uniaxial compression, indentation and dynamic mechanical analysis assay. Chondrocytes were then harvested from the knee joint of the New Zealand white rabbits and cultured in constructs. The cell proliferation, viability, production of glycosaminoglycans and collagen type II were assessed. The results showed that mechanical properties of the hydrogel were significantly enhanced when a hybrid with two layers of electrospun silk fibers was made. The results of GAG and collagen type II in cell-seeded scaffolds indicate support of the chondrogenic phenotype for chondrocytes with a significant increase in degummed silk fiber-hydrogel composite for GAG content and in two-layer electrospun fiber-hydrogel composite for Col II. It was concluded that these two modified scaffolds could be employed for cartilage tissue engineering. © 2013.

Modeling and simulation of a chemically stimulated hydrogel bilayer bending actuator

NASA Astrophysics Data System (ADS)

Sobczyk, Martin; Wallmersperger, Thomas

2017-04-01

Stimuli-sensitive hydrogels are polymeric materials, which are able to reversibly swell in water in response to evironmental changes. Relevant stimuli include variations of pH, temperature, concentration of specific ions etc. Stacked layers composed of multiple thin hydrogels - also referred to as hydrogel-layer composites - combine the distinct sensing properties of different hydrogels. This approach enables the development of sophisticated microfluidic devices such as bisensitive valves or fluid-sensitive deflectors. In order to numerically simulate the swelling of a polyelectrolyte hydrogel in response to an ion concentration change the multifield theory is adopted. The set of partial differential equations - including the description of the chemical, the electrical and the mechanical field - are solved using the Finite Element Method. Simulations are carried out on a two-dimensional domain in order to capture interactions between the different fields. In the present work, the ion transport is governed by diffusive and migrative fluxes. The distribution of ions in the gel and the solution bath result in an osmotic pressure difference, which is responsible for the mechanical deformation of the hydrogel-layer composite. The realized numerical investigation gives an insight into the evolution of the displacement field, the distribution of ions and the electric potential within the bulk material and the interface between gel and solution bath. The predicted behavior of the relevant field variables is in excellent agreement with results available in the literature.

Electrochemical immunoassay for tumor markers based on hydrogels.

PubMed

Yin, Shuang; Ma, Zhanfang

2018-05-08

Hydrogel-based electrochemical immunoassays exhibit a large surface-to-volume ratio, excellent biocompatibility, unique stimuli-responsive behavior, high permeability and hydrophilicity and, thus, have shown great potential in the sensitive and accurate detection of tumor markers. Electrochemical immunosensing techniques for tumor markers based on hydrogels have greatly progressed in recent years. Areas covered: In this review, the authors describe the recent advances of hydrogel-based electrochemical immunosensing interface of tumor markers based on the different functions of hydrogels including conductive, catalytic, redox, stimuli-responsive and antifouling hydrogels. Expert commentary: Hydrogels have been successfully employed in electrochemical immunoassay of tumor markers, which is accountable to their unique properties. For further exploitation of hydrogel-based electrochemical biosensors, more variety of hydrogels need be fabricated with improved functionality.

Multi-scale model for the hierarchical architecture of native cellulose hydrogels.

PubMed

Martínez-Sanz, Marta; Mikkelsen, Deirdre; Flanagan, Bernadine; Gidley, Michael J; Gilbert, Elliot P

2016-08-20

The structure of protiated and deuterated cellulose hydrogels has been investigated using a multi-technique approach combining small-angle scattering with diffraction, spectroscopy and microscopy. A model for the multi-scale structure of native cellulose hydrogels is proposed which highlights the essential role of water at different structural levels characterised by: (i) the existence of cellulose microfibrils containing an impermeable crystalline core surrounded by a partially hydrated paracrystalline shell, (ii) the creation of a strong network of cellulose microfibrils held together by hydrogen bonding to form cellulose ribbons and (iii) the differential behaviour of tightly bound water held within the ribbons compared to bulk solvent. Deuterium labelling provides an effective platform on which to further investigate the role of different plant cell wall polysaccharides in cellulose composite formation through the production of selectively deuterated cellulose composite hydrogels. Copyright © 2016 Elsevier Ltd. All rights reserved.

Effects of matrix composition, microstructure, and viscoelasticity on the behaviors of vocal fold fibroblasts cultured in three-dimensional hydrogel networks.

PubMed

Farran, Alexandra J E; Teller, Sean S; Jha, Amit K; Jiao, Tong; Hule, Rohan A; Clifton, Rodney J; Pochan, Darrin P; Duncan, Randall L; Jia, Xinqiao

2010-04-01

Vocal fold diseases and disorders are difficult to treat surgically or therapeutically. Tissue engineering offers an alternative strategy for the restoration of functional vocal folds. As a first step toward vocal fold tissue engineering, we investigated the responses of primary vocal fold fibroblasts (PVFFs) to two types of collagen and hyaluronic acid (HA)-based hydrogels that are compositionally similar, but structurally variable and mechanically different. Type A hydrogels were composed of mature collagen fibers reinforced by oxidized HA, whereas type B hydrogels contained immature collagen fibrils interpenetrated in an amorphous, covalently cross-linked HA matrix. PVFFs encapsulated in either matrix adopted a fibroblastic morphology and expressed genes related to important extracellular matrix proteins. DNA analysis indicated a linear growth profile for cells encapsulated in type B gels from day 0 to 21, in contrast to an initial dormant, nonproliferative period from day 0 to 3 experienced by cells in type A gels. At the end of the culture, similar DNA content was detected in both types of constructs. A reduction in collagen content was observed for both types of constructs after 28 days of culture, with type A constructs generally retaining higher amounts of collagen than type B constructs. The HA content in the constructs decreased steadily throughout the culture, with type A constructs consistently exhibiting less HA than type B constructs. Using the torsional wave analysis, we found that the elastic moduli for type A constructs decreased sharply during the first week of culture, followed by 2 weeks of matrix stabilization without significant changes in matrix stiffness. Conversely, the elastic modulus for type B constructs increased moderately over time. It is postulated that PVFFs residing in gels alter the matrix organization, chemical compositions, and viscoelasticity through cell-mediated remodeling processes.

Flexible Asymmetric Supercapacitors Based on Nitrogen-Doped Graphene Hydrogels with Embedded Nickel Hydroxide Nanoplates.

PubMed

Xie, Hao; Tang, Shaochun; Li, Dongdong; Vongehr, Sascha; Meng, Xiangkang

2017-05-22

To push the energy density limit of supercapacitors (SCs), new electrode materials with hierarchical nano-micron pore architectures are strongly desired. Graphene hydrogels that consist of 3 D porous frameworks have received particular attention but their capacitance is limited by electrical double layer capacitance. In this work, we report the rational design and fabrication of a composite hydrogel of N-doped graphene (NG) that contains embedded Ni(OH) 2 nanoplates that is cut conveniently into films to serve as positive electrodes for flexible asymmetric solid-state SCs with NG hydrogel films as negative electrodes. The use of high-power ultrasound leads to hierarchically porous micron-scale sheets that consist of a highly interconnected 3 D NG network in which Ni(OH) 2 nanoplates are well dispersed, which avoids the stacking of NG, Ni(OH) 2 , and their composites. The optimal SC device benefits from the compositional features and 3 D electrode architecture and has a high specific areal capacitance of 255 mF cm -2 at 1.0 mA cm -2 and a very stable, high output cell voltage of 1.45 V, which leads to an energy density of 80 μW h cm -2 even at a high power of 944 μW cm -2 , considerably higher than that reported for similar devices. The devices exhibit a high rate capability and only 8 % capacitance loss over 10 000 charging cycles as well as excellent flexibility with no clear performance degradation under strong bending. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tunable hydrogel composite with two-step processing in combination with innovative hardware upgrade for cell-based three-dimensional bioprinting.

PubMed

Wüst, Silke; Godla, Marie E; Müller, Ralph; Hofmann, Sandra

2014-02-01

Three-dimensional (3-D) bioprinting is the layer-by-layer deposition of biological material with the aim of achieving stable 3-D constructs for application in tissue engineering. It is a powerful tool for the spatially directed placement of multiple materials and/or cells within the 3-D sample. Encapsulated cells are protected by the bioink during the printing process. Very few materials are available that fulfill requirements for bioprinting as well as provide adequate properties for cell encapsulation during and after the printing process. A hydrogel composite including alginate and gelatin precursors was tuned with different concentrations of hydroxyapatite (HA) and characterized in terms of rheology, swelling behavior and mechanical properties to assess the versatility of the system. Instantaneous as well as long-term structural integrity of the printed hydrogel was achieved with a two-step mechanism combining the thermosensitive properties of gelatin with chemical crosslinking of alginate. Novel syringe tip heaters were developed for improved temperature control of the bioink to avoid clogging. Human mesenchymal stem cells mixed into the hydrogel precursor survived the printing process and showed high cell viability of 85% living cells after 3 days of subsequent in vitro culture. HA enabled the visualization of the printed structures with micro-computed tomography. The inclusion of HA also favors the use of the bioink for bone tissue engineering applications. By adding factors other than HA, the composite could be used as a bioink for applications in drug delivery, microsphere deposition or soft tissue engineering. Copyright © 2013 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Effect of Chemical Washing Pre-treatment of Empty Fruit Bunch (EFB) biochar on Characterization of Hydrogel Biochar composite as Bioadsorbent

NASA Astrophysics Data System (ADS)

Meri, N. H.; Alias, A. B.; Talib, N.; Rashid, Z. A.; Wan, W. A.; Ghani, Ab Karim

2018-05-01

Hydrogel biochar composite (HBC) is a recent interest among researchers because of the hydrophilic characteristic which can adsorb chemical fluid and showed a versatile potential as adsorbent in removing hazardous material in wastewater and gas stream. In this study, the effect of chemical washing pre-treatment by using two different type of chemical agent Hydrochloric Acid (HCL) and Hydrogen Peroxide (H2O2) was analysed and investigated. The raw EFB biochar was prepared using microwave assisted pyrolysis under 1000W for 30 min under N2 flow with 150 mL/min. To improve the adsoprtion ability, the EFB biochar has been chemical washed pre-treatment with Hydrochloric Acid (HCl) and Hydrogen Peroxide (H2O2) before polymerization process with acrylamide (AAm) as monomer, N,N’-methylenebisacrylamide (MBA) as crosslinker and ammonium persulfate (APS) as initiator. The characterization has studied by using Fourier transform infrared spectroscopy (FTIR) and Differential Scanning Calorimetry (DSC). FTIR result shows that, the formation of Raw EFB to Hydrogel Biochar Composite (Raw EFB > EFB Biochar > Treated Biochars (HCl & H2O2) > Hydrogel Biochar Composite) have changed in functional group. For DSC result it shows that the thermal behaviour of all samples is endothermic process and have high thermal resistance.

A simple route to synthesize conductive stimuli-responsive polypyrrole nanocomposite hydrogel particles with strong magnetic properties and their performance for removal of hexavalent chromium ions from aqueous solution

NASA Astrophysics Data System (ADS)

Ahmad, Hasan; Rahman, Mohammad Mostafizar; Ali, Mohammad Azgar; Minami, Hideto; Tauer, Klaus; Gafur, Mohammad Abdul; Rahman, Mohammad Mahbubor

2016-08-01

A combination of maghemite polypyrrole (PPy/γ-Fe2O3) and stimuli-responsive properties in the same hydrogel microspheres is expected to enhance their application potential in various fields such as tissue engineering, regenerative medicine, biosensors, biomedical applications and removal of heavy metals from waste water, catalysis etc. In this investigation a simple two step process is used to prepare conductive stimuli-responsive polypyrrole (PPy) composite hydrogel particles with strong magnetic properties. Poly(styrene-methacrylic acid-N-isopropylacrylamide-polyethelene glycol methacrylate) or P(S-NIPAM-MAA-PEGMA) hydrogel seed particles are first prepared by soap-free precipitation copolymerization. The copolymer hydrogel particles exhibited both temperature- and pH-responsive volume phase transition. Conductive P(S-NIPAM-MAA-PEGMA)/PPy/γ-Fe2O3 nanocomposite hydrogel particles are then prepared by seeded chemical oxidative polymerization of pyrrole in the presence of P(S-NIPAM-MAA-PEGMA) hydrogel seed particles using FeCl3 as a oxidant and p-toluene sulfonic acid (p-TSA) as a dopant. In the reaction system FeCl3 functioned as a source of Fe(III) for the formation of γ-Fe2O3. This reaction also requires the initial presence of Fe(II) provided by the addition of FeCl2. The size and size distribution, surface structure, and morphology of the prepared conductive composite hydrogel particles are confirmed by FTIR, electron micrographs, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and UV-visible spectroscopy. The performance of nanocomposite hydrogel particles has been evaluated for the removal of hexavalent chromium (Cr) ions from water.

Human umbilical cord blood-derived mesenchymal stromal cells and small intestinal submucosa hydrogel composite promotes combined radiation-wound healing of mice.

PubMed

Lee, Changsun; Shim, Sehwan; Jang, Hyosun; Myung, Hyunwook; Lee, Janet; Bae, Chang-Hwan; Myung, Jae Kyung; Kim, Min-Jung; Lee, Seung Bum; Jang, Won-Suk; Lee, Sun-Joo; Kim, Hwi-Yool; Lee, Seung-Sook; Park, Sunhoo

2017-09-01

Mesenchymal stromal cells (MSCs) are a promising agent for treating impaired wound healing, and their therapeutic potential may be enhanced by employing extracellular matrix scaffolds as cell culture scaffolds or transplant cell carriers. Here, we evaluated the effect of human umbilical cord blood-derived (hUCB)-MSCs and a porcine small intestinal submucosa (SIS)-derived extracellular matrix scaffold in a combined radiation-wound mouse model of impaired wound healing. hUCB-MSCs and SIS hydrogel composite was applied to the excisional wound of whole-body irradiated mice. Assessment of wound closing and histological evaluation were performed in vivo. We also cultured hUCB-MSCs on SIS gel and examined the angiogenic effect of conditioned medium on irradiated human umbilical vein endothelial cells (HUVECs) in vitro. hUCB-MSCs and SIS hydrogel composite treatment enhanced wound healing and angiogenesis in the wound site of mice. Conditioned medium from hUCB-MSCs cultured on SIS hydrogel promoted the chemotaxis of irradiated HUVECs more than their proliferation. The secretion of angiogenic growth factors hepatocyte growth factor, vascular endothelial growth factor-A and angiopoietin-1 from hUCB-MSCs was significantly increased by SIS hydrogel, with HGF being the predominant angiogenic factor of irradiated HUVECs. Our results suggest that the wound healing effect of hUCB-MSCs is enhanced by SIS hydrogel via a paracrine factor-mediated recruitment of vascular endothelial cells in a combined radiation-wound mouse model. Copyright © 2017 International Society for Cellular Therapy. Published by Elsevier Inc. All rights reserved.

Biodestruction of strongly swelling polymer hydrogels and its effect on the water retention capacity of soils

NASA Astrophysics Data System (ADS)

Smagin, A. V.; Sadovnikova, N. B.; Smagina, M. V.

2014-06-01

The biodestruction of strongly swelling polymer hydrogels (water adsorbing soil conditioners of the new generation) has been studied at the quantitative level using original mathematical models. In laboratory experiments, a relationship between the hydrogel degradation rate and the temperature has been obtained, and the effect of the biodestruction on the water retention curve of soil compositions with hydrogels (used as an index of their water retention capacity) has been assessed. From the automatic monitoring data of the temperature regime of soils, the potential biodestruction of hydrogels has been predicted for different climatic conditions. The loss of hydrogels during three months of the vegetation period because of destruction can exceed 30% of their initial content in irrigated agriculture under arid climatic conditions and more than 10% under humid climatic conditions. Thus, the biodestruction of hydrogels is one of the most important factors decreasing their efficiency under actual soil conditions.

Thermogelling chitosan and collagen composite hydrogels initiated with β-glycerophosphate for bone tissue engineering

PubMed Central

Wang, Limin; Stegemann, Jan P.

2010-01-01

Chitosan and collagen type I are naturally-derived materials used as cell carriers because of their ability to mimic the extracellular environment and direct cell function. In this study beta-glycerophosphate (beta-GP), an osteogenic medium supplement and a weak base, was used to simultaneously initiate gelation of pure chitosan, pure collagen, and chitosan-collagen composite materials at physiological pH and temperature. Adult human bone marrow-derived stem cells (hBMSC) encapsulated in such hydrogels at chitosan/collagen ratios of 100/0, 65/35, 25/75, and 0/100 wt% exhibited high viability at day 1 after encapsulation, but DNA content dropped by about half over 12 days in pure chitosan materials while it increased two-fold in materials containing collagen. Collagen-containing materials compacted more strongly and were significantly stiffer than pure chitosan gels. In monolayer culture, exposure of hBMSC to beta-GP resulted in decreased cell metabolic activity that varied with concentration and exposure time, but washing effectively removed excess beta-GP from hydrogels. The presence of chitosan in materials resulted in higher expression of osterix and bone sialoprotein genes in medium with and without osteogenic supplements. Chitosan also increased alkaline phosphatase activity and calcium deposition in osteogenic medium. Chitosan-collagen composite materials have potential as matrices for cell encapsulation and delivery, or as in situ gel-forming materials for tissue repair. PMID:20170955

Thermogelling chitosan and collagen composite hydrogels initiated with beta-glycerophosphate for bone tissue engineering.

PubMed

Wang, Limin; Stegemann, Jan P

2010-05-01

Chitosan and collagen type I are naturally derived materials used as cell carriers because of their ability to mimic the extracellular environment and direct cell function. In this study beta-glycerophosphate (beta-GP), an osteogenic medium supplement and a weak base, was used to simultaneously initiate gelation of pure chitosan, pure collagen, and chitosan-collagen composite materials at physiological pH and temperature. Adult human bone marrow-derived stem cells (hBMSC) encapsulated in such hydrogels at chitosan/collagen ratios of 100/0, 65/35, 25/75, and 0/100 wt% exhibited high viability at day 1 after encapsulation, but DNA content dropped by about half over 12 days in pure chitosan materials while it increased twofold in materials containing collagen. Collagen-containing materials compacted more strongly and were significantly stiffer than pure chitosan gels. In monolayer culture, exposure of hBMSC to beta-GP resulted in decreased cell metabolic activity that varied with concentration and exposure time, but washing effectively removed excess beta-GP from hydrogels. The presence of chitosan in materials resulted in higher expression of osterix and bone sialoprotein genes in medium with and without osteogenic supplements. Chitosan also increased alkaline phosphatase activity and calcium deposition in osteogenic medium. Chitosan-collagen composite materials have potential as matrices for cell encapsulation and delivery, or as in situ gel-forming materials for tissue repair. Copyright 2010 Elsevier Ltd. All rights reserved.

Carbon Nanotubes Hybrid Hydrogels in Drug Delivery: A Perspective Review

PubMed Central

Hampel, Silke; Spizzirri, Umile Gianfranco; Parisi, Ortensia Ilaria; Picci, Nevio; Iemma, Francesca

2014-01-01

The use of biologics, polymers, silicon materials, carbon materials, and metals has been proposed for the preparation of innovative drug delivery devices. One of the most promising materials in this field are the carbon-nanotubes composites and hybrid materials coupling the advantages of polymers (biocompatibility and biodegradability) with those of carbon nanotubes (cellular uptake, stability, electromagnatic, and magnetic behavior). The applicability of polymer-carbon nanotubes composites in drug delivery, with particular attention to the controlled release by composites hydrogel, is being extensively investigated in the present review. PMID:24587993

A novel strategy towards designing a CdSe quantum dot-metallohydrogel composite material.

PubMed

Chatterjee, Sayantan; Maitra, Uday

2016-08-11

We have described here an efficient method to disperse hydrophobic CdSe quantum dots (QDs) in an aqueous phase using cetyltrimethylammonium bromide (CTAB) micelles without any surface ligand exchange. The water soluble QDs were then embedded in 3D self assembled fibrillar networks (SAFINs) of a hydrogel showing homogeneous dispersibility as evidenced from optical and electron microscopic techniques. The photophysical studies of the hydrogel-QD composite are reported for the first time. These composite materials may have potential applications in biology, optoelectronics, sensors, non-linear optics and materials science.

Novel synthesis strategy for composite hydrogel of collagen/hydroxyapatite-microsphere originating from conversion of CaCO3 templates.

PubMed

Wei, Qingrong; Lu, Jian; Wang, Qiaoying; Fan, Hongsong; Zhang, Xingdong

2015-03-20

Inspired by coralline-derived hydroxyapatite, we designed a methodological route to synthesize carbonated-hydroxyapatite microspheres from the conversion of CaCO3 spherulite templates within a collagen matrix under mild conditions and thus constructed the composite hydrogel of collagen/hydroxyapatite-microspheres. Fourier transform infrared spectroscopy (FTIR) and x-ray diffraction (XRD) were employed to confirm the successful generation of the carbonated hydroxyapatite phase originating from CaCO3, and the ratios of calcium to phosphate were tracked over time. Variations in the weight portion of the components in the hybrid gels before and after the phase transformation of the CaCO3 templates were identified via thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) shows these composite hydrogels have a unique multiscale microstructure consisting of a collagen nanofibril network and hydroxyapatite microspheres. The relationship between the hydroxyapatite nanocrystals and the collagen fibrils was revealed by transmission electron microscopy (TEM) in detail, and the selected area electron diffraction (SAED) pattern further confirmed the results of the XRD analyses which show the typical low crystallinity of the generated hydroxyapatite. This smart synthesis strategy achieved the simultaneous construction of microscale hydroxyapatite particles and collagen fibrillar hydrogel, and appears to provide a novel route to explore an advanced functional hydrogel materials with promising potentials for applications in bone tissue engineering and reconstruction medicine.

Adsorption of Heavy Metals by Graphene Oxide/Cellulose Hydrogel Prepared from NaOH/Urea Aqueous Solution

PubMed Central

Chen, Xiong; Zhou, Sukun; Zhang, Liming; You, Tingting; Xu, Feng

2016-01-01

By taking advantage of cellulose, graphene oxide (GO), and the process for crosslinking using epichlorohydrin (ECH), we propose a simple and novel method to prepare GO/cellulose hydrogel with good potential to adsorb metal ions. GO nanosheets containing carboxyl and hydroxyl groups were introduced into the surface of the cellulose hydrogel with retention of the gel structure and its nanoporous property. Due to the introduction of GO, the GO/cellulose composite hydrogels exhibited good compressive strength. Adsorption capacity of Cu2+ significantly increases with an increase in the GO/cellulose ratio and GO/cellulose hydrogel showed high adsorption rates. The calculated adsorption capacities at equilibrium (qecal) for GO/cellulose hydrogel (GO:cellulose = 20:100 in weight) was up to 94.34 mg·g−1, which was much higher than that of the pristine cellulose hydrogels. Furthermore, GO/cellulose hydrogel exhibited high efficient regeneration and metal ion recovery, and high adsorption capacity for Zn2+, Fe3+, and Pb2+. PMID:28773705

Skin-Inspired Hydrogel-Elastomer Composite with Application in a Moisture Permeable Prosthetic Limb Liner

NASA Astrophysics Data System (ADS)

Ruiz, Esteban

Recent advances in fields such as 3D printing, and biomaterials, have enabled the development of a moisture permeable prosthetic liner. This project demonstrates the feasibility of the invention by addressing the three primary areas of risk including the mechanical strength, the permeability, and the ability to manufacture. The key enabling technology which allows the liner to operate is the skin inspired hydrogel elastomer composite. The skin inspiration is reflected in the molecular arrangement of the double network of polymers which mimics collagen-elastin toughening in the natural epidermis. A custom formulation for a novel tough double network nanocomposite reinforced hydrogel was developed to improve manufacturability of the liner. The liner features this double network nanocomposite reinforced hydrogel as a permeable membrane which is reinforced on either side by perforated silicone layers manufactured by 3d printing assisted casting. Uniaxial compression tests were conducted on the individual hydrogels, as well as a representative sample of off the shelf prosthetic liners for comparison. Permeability testing was also done on the same set of materials and compared to literature values for traditional hydrogels. This work led to the manufacture of three generations of liner prototypes, with the second and third liner prototype being tested with human participants.

Salmonella enterica biofilm-mediated dispersal by nitric oxide donors in association with cellulose nanocrystal hydrogels.

PubMed

Marvasi, Massimiliano; Durie, Ian A; McLamore, Eric S; Vanegas, Diana C; Chaturvedi, Prachee

2015-01-01

Protected by extracellular polymers, microbes within biofilms are significantly more resistant to disinfectants. Current research has been instrumental in identifying nitric oxide donors and hydrogels as potential disinfectant additives. Nitric oxide (NO) donors are considered a very promising molecule as biofilm dispersal agents and hydrogels have recently attracted a lot of interest due to their biocompatible properties and ability to form stable thin films. When the NO donor MAHMA NONOate was dissolved in phosphate saline buffer, it was able to reduce the biomass of well-established biofilms up to 15% for at least 24 h of contact time. Encapsulation of MAHMA NONOate and molsidomine within a hydrogel composed of cellulose nanocrystals (CNC) has shown a synergistic effect in dispersing well-established biofilms: after 2 h of exposure, moderate but significant dispersion was measured. After 6 h of exposure, the number of cells transitioning from the biofilm to the planktonic state was up to 0.6 log higher when compared with non-treated biofilms. To further explore the transport processes of NO donors within hydrogels, we measured the nitric oxide flux from gels, at 25°C for a composite of 0.1 µM MAHMA NONOate-CNC. Nitric oxide diffuses up to 500 µm from the hydrogel surface, with flux decreasing according to Fick's law. 60% of NO was released from the hydrogel composite during the first 23 min. These data suggest that the combined treatments with nitric oxide donor and hydrogels may allow for new sustainable cleaning strategies.

In vitro-ex vivo correlations between a cell-laden hydrogel and mucosal tissue for screening composite delivery systems

PubMed Central

Blakney, Anna K.; Little, Adam B.; Jiang, Yonghou; Woodrow, Kim A.

2017-01-01

Composite delivery systems where drugs are electrospun in different layers and vary the drug stacking-order are posited to affect bioavailability. We evaluated how the formulation characteristics of both burst- and sustained-release electrospun fibers containing three physicochemically diverse drugs: dapivirine (DPV), maraviroc (MVC) and tenofovir (TFV) affect in vitro and ex vivo release. We developed a poly(hydroxyethyl methacrylate) (pHEMA) hydrogel release platform for the rapid, inexpensive in vitro evaluation of burst- and sustained-release topical or dermal drug delivery systems with varying microarchitecture. We investigated properties of the hydrogel that could recapitulate ex vivo release into nonhuman primate vaginal tissue. Using a DMSO extraction protocol and HPLC analysis, we achieved >93% recovery from the hydrogels and >88% recovery from tissue explants for all three drugs. We found that DPV loading, but not stacking order (layers of fiber containing a single drug) or microarchitecture (layers with isolated drug compared to all drugs in the same layer) impacted the burst release in vitro and ex vivo. Our burst-release formulations showed a correlation for DPV accumulation between the hydrogel and tissue (R2=0.80), but the correlation was not significant for MVC or TFV. For the sustained release formulations, the PLGA/PCL content did not affect TFV release in vitro or ex vivo. Incorporation of cells into the hydrogel matrix improved the correlation between hydrogel and tissue explant release for TFV. We expect that this hydrogel tissue mimic maybe a promising preclinical model to evaluate topical or transdermal drug delivery systems with complex microarchitectures. PMID:28222612

A comparison of different bioinks for 3D bioprinting of fibrocartilage and hyaline cartilage.

PubMed

Daly, Andrew C; Critchley, Susan E; Rencsok, Emily M; Kelly, Daniel J

2016-10-07

Cartilage is a dense connective tissue with limited self-repair capabilities. Mesenchymal stem cell (MSC) laden hydrogels are commonly used for fibrocartilage and articular cartilage tissue engineering, however they typically lack the mechanical integrity for implantation into high load bearing environments. This has led to increased interested in 3D bioprinting of cell laden hydrogel bioinks reinforced with stiffer polymer fibres. The objective of this study was to compare a range of commonly used hydrogel bioinks (agarose, alginate, GelMA and BioINK™) for their printing properties and capacity to support the development of either hyaline cartilage or fibrocartilage in vitro. Each hydrogel was seeded with MSCs, cultured for 28 days in the presence of TGF-β3 and then analysed for markers indicative of differentiation towards either a fibrocartilaginous or hyaline cartilage-like phenotype. Alginate and agarose hydrogels best supported the development of hyaline-like cartilage, as evident by the development of a tissue staining predominantly for type II collagen. In contrast, GelMA and BioINK ™ (a PEGMA based hydrogel) supported the development of a more fibrocartilage-like tissue, as evident by the development of a tissue containing both type I and type II collagen. GelMA demonstrated superior printability, generating structures with greater fidelity, followed by the alginate and agarose bioinks. High levels of MSC viability were observed in all bioinks post-printing (∼80%). Finally we demonstrate that it is possible to engineer mechanically reinforced hydrogels with high cell viability by co-depositing a hydrogel bioink with polycaprolactone filaments, generating composites with bulk compressive moduli comparable to articular cartilage. This study demonstrates the importance of the choice of bioink when bioprinting different cartilaginous tissues for musculoskeletal applications.

Hydrogel-Based Fluorescent Dual pH and Oxygen Sensors Loaded in 96-Well Plates for High-Throughput Cell Metabolism Studies.

PubMed

Wu, Shanshan; Wu, Siying; Yi, Zheyuan; Zeng, Fei; Wu, Weizhen; Qiao, Yuan; Zhao, Xingzhong; Cheng, Xing; Tian, Yanqing

2018-02-13

In this study, we developed fluorescent dual pH and oxygen sensors loaded in multi-well plates for in-situ and high-throughput monitoring of oxygen respiration and extracellular acidification during microbial cell growth for understanding metabolism. Biocompatible PHEMA-co-PAM materials were used as the hydrogel matrix. A polymerizable oxygen probe (OS2) derived from PtTFPP and a polymerizable pH probe (S2) derived from fluorescein were chemically conjugated into the matrix to solve the problem of the probe leaching from the matrix. Gels were allowed to cure directly on the bottom of 96-well plates at room-temperature via redox polymerization. The influence of matrix's composition on the sensing behaviors was investigated to optimize hydrogels with enough robustness for repeatable use with good sensitivity. Responses of the dual sensing hydrogels to dissolved oxygen (DO) and pH were studied. These dual oxygen-pH sensing plates were successfully used for microbial cell-based screening assays, which are based on the measurement of fluorescence intensity changes induced by cellular oxygen consumption and pH changes during microbial growth. This method may provide a real-time monitoring of cellular respiration, acidification, and a rapid kinetic assessment of multiple samples for cell viability as well as high-throughput drug screening. All of these assays can be carried out by a conventional plate reader.

Injectable polypeptide hydrogels via methionine modification for neural stem cell delivery.

PubMed

Wollenberg, A L; O'Shea, T M; Kim, J H; Czechanski, A; Reinholdt, L G; Sofroniew, M V; Deming, T J

2018-04-05

Injectable hydrogels with tunable physiochemical and biological properties are potential tools for improving neural stem/progenitor cell (NSPC) transplantation to treat central nervous system (CNS) injury and disease. Here, we developed injectable diblock copolypeptide hydrogels (DCH) for NSPC transplantation that contain hydrophilic segments of modified l-methionine (Met). Multiple Met-based DCH were fabricated by post-polymerization modification of Met to various functional derivatives, and incorporation of different amino acid comonomers into hydrophilic segments. Met-based DCH assembled into self-healing hydrogels with concentration and composition dependent mechanical properties. Mechanical properties of non-ionic Met-sulfoxide formulations (DCH MO ) were stable across diverse aqueous media while cationic formulations showed salt ion dependent stiffness reduction. Murine NSPC survival in DCH MO was equivalent to that of standard culture conditions, and sulfoxide functionality imparted cell non-fouling character. Within serum rich environments in vitro, DCH MO was superior at preserving NSPC stemness and multipotency compared to cell adhesive materials. NSPC in DCH MO injected into uninjured forebrain remained local and, after 4 weeks, exhibited an immature astroglial phenotype that integrated with host neural tissue and acted as cellular substrates that supported growth of host-derived axons. These findings demonstrate that Met-based DCH are suitable vehicles for further study of NSPC transplantation in CNS injury and disease models. Copyright © 2018 Elsevier Ltd. All rights reserved.

Controlled drug delivery through a novel PEG hydrogel encapsulated silica aerogel system.

PubMed

Giray, Seda; Bal, Tuğba; Kartal, Ayse M; Kızılel, Seda; Erkey, Can

2012-05-01

A novel composite material consisting of a silica aerogel core coated by a poly(ethylene) glycol (PEG) hydrogel was developed. The potential of this novel composite as a drug delivery system was tested with ketoprofen as a model drug due to its solubility in supercritical carbon dioxide. The results indicated that both drug loading capacity and drug release profiles could be tuned by changing hydrophobicity of aerogels, and that drug loading capacity increased with decreased hydrophobicity, while slower release rates were achieved with increased hydrophobicity. Furthermore, higher concentration of PEG diacrylate in the prepolymer solution of the hydrogel coating delayed the release of the drug which can be attributed to the lower permeability at higher PEG diacrylate concentrations. The novel composite developed in this study can be easily implemented to achieve the controlled delivery of various drugs and/or proteins for specific applications. Copyright © 2012 Wiley Periodicals, Inc.

Development of a self-cleaning sensor membrane for implantable biosensors.

PubMed

Gant, Rebecca M; Hou, Yaping; Grunlan, Melissa A; Coté, Gerard L

2009-09-01

Fibrous tissue encapsulation may slow the diffusion of the target analyte to an implanted sensor and compromise the optical signal. Poly(N-isopropylacrylamide) (PNIPAAm) hydrogels are thermoresponsive, exhibiting temperature-modulated swelling behavior that could be used to prevent biofouling. Unfortunately, PNIPAAm hydrogels are limited by poor mechanical strength. In this study, a unique thermoresponsive nanocomposite hydrogel was developed to create a mechanically robust self-cleaning sensor membrane for implantable biosensors. This hydrogel was prepared by the photochemical cure of an aqueous solution of NIPAAm and copoly(dimethylsiloxane/methylvinylsiloxane) colloidal nanoparticles ( approximately 219 nm). At temperatures above the volume phase transition temperature (VPTT) of approximately 33-34 degrees C, the hydrogel deswells and becomes hydrophobic, whereas lowering the temperature below the VPTT causes the hydrogel to swell and become hydrophilic. The potential of this material to minimize biofouling via temperature-modulation while maintaining sensor viability was investigated using glucose as a target analyte. PNIPAAm composite hydrogels with and without poration were compared to a pure PNIPAAm hydrogel and a nonthermoresponsive poly(ethylene glycol) (PEG) hydrogel. Poration led to a substantial increase in diffusion. Cycling the temperature of the nanocomposite hydrogels around the VPTT caused significant detachment of GFP-H2B 3T3 fibroblast cells.

An integrated system for dissolution studies and magnetic resonance imaging of controlled release, polymer-based dosage forms-a tool for quantitative assessment of hydrogel formation processes.

PubMed

Kulinowski, Piotr; Dorozyński, Przemysław; Jachowicz, Renata; Weglarz, Władysław P

2008-11-04

Controlled release (CR) dosage forms are often based on polymeric matrices, e.g., sustained-release tablets and capsules. It is crucial to visualise and quantify processes of the hydrogel formation during the standard dissolution study. A method for imaging of CR, polymer-based dosage forms during dissolution study in vitro is presented. Imaging was performed in a non-invasive way by means of the magnetic resonance imaging (MRI). This study was designed to simulate in vivo conditions regarding temperature, volume, state and composition of dissolution media. Two formulations of hydrodynamically balanced systems (HBS) were chosen as model CR dosage forms. HBS release active substance in stomach while floating on the surface of the gastric content. Time evolutions of the diffusion region, hydrogel formation region and "dry core" region were obtained during a dissolution study of L-dopa as a model drug in two simulated gastric fluids (i.e. in fed and fasted state). This method seems to be a very promising tool for examining properties of new formulations of CR, polymer-based dosage forms or for comparison of generic and originator dosage forms before carrying out bioequivalence studies.

Material and fabrication strategies for artificial muscles (Conference Presentation)

NASA Astrophysics Data System (ADS)

Spinks, Geoffrey M.

2017-04-01

Soft robotic and wearable robotic devices seek to exploit polymer based artificial muscles and sensor materials to generate biomimetic movements and forces. A challenge is to integrate the active materials into a complex, three-dimensional device with integrated electronics, power supplies and support structures. Both 3D printing and textiles technologies offer attractive fabrication strategies, but require suitable functional materials. 3D printing of actuating hydrogels has been developed to produce simple devices, such as a prototype valve. Tough hydrogels based on interpenetrating networks of ionicially crosslinked alginate and covalently crosslinked polyacrylamide and poly(N-isopropylacrylamide) have been developed in a form suitable for extrusion printing with UV curing. Combined with UV-curable and extrudable rigid acrylated urethanes, the tough hydrogels can be 3D printed into composite materials or complex shapes with multiple different materials. An actuating valve was printed that operated thermally to open or close the flow path using 6 parallel hydrogel actuators. Textile processing methods such as knitting and weaving can be used to generate assemblies of actuating fibres. Low cost and high performance coiled fibres made from oriented polymers have been used for developing actuating textiles. Similarly, braiding methods have been developed to fabricate new forms of McKibben muscles that operate without any external apparatus, such as pumps, compressors or piping.

Enzyme-mediated hyaluronic acid-tyramine hydrogels for the propagation of human embryonic stem cells in 3D.

PubMed

Xu, Keming; Narayanan, Karthikeyan; Lee, Fan; Bae, Ki Hyun; Gao, Shujun; Kurisawa, Motoichi

2015-09-01

The propagation of human embryonic stem cells (hESCs) in three-dimensional (3D) scaffolds facilitates the cell expansion process and supplies pluripotent cells of high quality for broad-spectrum applications in regenerative medicine. Herein, we report an enzyme-mediated hyaluronic acid-tyramine (HA-Tyr) hydrogel that encapsulated and propagated hESCs in 3D. HA-Tyr hydrogels were formed by crosslinking the tyramine moieties with horseradish peroxidase (HRP) and hydrogen peroxide (H2O2). By changing the HRP and H2O2 concentration, we prepared HA-Tyr hydrogels of different mechanical strength and studied the self-renewal properties of hESCs in these scaffolds. We observed that both the chemical composition and mechanical strength of substrates were important factors affecting cell proliferation and pluripotency. The HA-Tyr hydrogel with a compressive modulus of ∼350Pa supported the proliferation of hESCs at the pluripotent state in both mTeSR1 medium and mouse embryonic fibroblast (MEF)-conditioned medium. Immunohistochemical analyses revealed that hESCs proliferated well and formed spheroid structures in 3D, without undergoing apoptosis. The hESCs cultured in HA-Tyr hydrogels showed high expression of CD44 and pluripotency markers. These cells exhibited the capability to form cell derivatives of all three embryonic germ layers in vitro and in vivo. In addition, the genetic integrity of the hESCs was unaffected in the 3D cultivation system. The scope of this study is to provide a stable 3D cultivation system for the expansion of human embryonic stem cells (hESCs) towards clinical applications. We report an enzyme mediated hyaluronic acid-tyramine (HA-Tyr) hydrogel that encapsulated and propagated hESCs in 3D. Unlike other HA-based photo-crosslinked hydrogel systems reported, we investigated the effects of mechanical strength of hydrogels on the self-renewal properties of hESCs in 3D. Then, we characterized hESCs cultured in hydrogels with lower mechanical strength that best supported the self-renewal of hESCs. Hence, we demonstrated a reliable approach for the controlled propagation of hESCs in 3D. We believe that such an approach would facilitate the development of stem cell-based therapy towards clinical applications. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Hydrogels for precision meniscus tissue engineering: a comprehensive review.

PubMed

Rey-Rico, Ana; Cucchiarini, Magali; Madry, Henning

The meniscus plays a pivotal role to preserve the knee joint homeostasis. Lesions to the meniscus are frequent, have a reduced ability to heal, and may induce tibiofemoral osteoarthritis. Current reconstructive therapeutic options mainly focus on the treatment of lesions in the peripheral vascularized region. In contrast, few approaches are capable of stimulating repair of damaged meniscal tissue in the central, avascular portion. Tissue engineering approaches are of high interest to repair or replace damaged meniscus tissue in this area. Hydrogel-based biomaterials are of special interest for meniscus repair as its inner part contains relatively high proportions of proteoglycans which are responsible for the viscoelastic compressive properties and hydration grade. Hydrogels exhibiting high water content and providing a specific three-dimensional (3D) microenvironment may be engineered to precisely resemble this topographical composition of the meniscal tissue. Different polymers of both natural and synthetic origins have been manipulated to produce hydrogels hosting relevant cell populations for meniscus regeneration and provide platforms for meniscus tissue replacement. So far, these compounds have been employed to design controlled delivery systems of bioactive molecules involved in meniscal reparative processes or to host genetically modified cells as a means to enhance meniscus repair. This review describes the most recent advances on the use of hydrogels as platforms for precision meniscus tissue engineering.

Bioreactor mechanically guided 3D mesenchymal stem cell chondrogenesis using a biocompatible novel thermo-reversible methylcellulose-based hydrogel.

PubMed

Cochis, A; Grad, S; Stoddart, M J; Farè, S; Altomare, L; Azzimonti, B; Alini, M; Rimondini, L

2017-03-23

Autologous chondrocyte implantation for cartilage repair represents a challenge because strongly limited by chondrocytes' poor expansion capacity in vitro. Mesenchymal stem cells (MSCs) can differentiate into chondrocytes, while mechanical loading has been proposed as alternative strategy to induce chondrogenesis excluding the use of exogenous factors. Moreover, MSC supporting material selection is fundamental to allow for an active interaction with cells. Here, we tested a novel thermo-reversible hydrogel composed of 8% w/v methylcellulose (MC) in a 0.05 M Na 2 SO 4 solution. MC hydrogel was obtained by dispersion technique and its thermo-reversibility, mechanical properties, degradation and swelling were investigated, demonstrating a solution-gelation transition between 34 and 37 °C and a low bulk degradation (<20%) after 1 month. The lack of any hydrogel-derived immunoreaction was demonstrated in vivo by mice subcutaneous implantation. To induce in vitro chondrogenesis, MSCs were seeded into MC solution retained within a porous polyurethane (PU) matrix. PU-MC composites were subjected to a combination of compression and shear forces for 21 days in a custom made bioreactor. Mechanical stimulation led to a significant increase in chondrogenic gene expression, while histological analysis detected sulphated glycosaminoglycans and collagen II only in loaded specimens, confirming MC hydrogel suitability to support load induced MSCs chondrogenesis.

High performances of dual network PVA hydrogel modified by PVP using borax as the structure-forming accelerator

PubMed Central

Huang, Min; Hou, Yi; Li, Yubao; Wang, Danqing; Zhang, Li

2017-01-01

Abstract A dual network hydrogel made up of polyvinylalcohol (PVA) crosslinked by borax and polyvinylpyrrolidone (PVP) was prepared by means of freezing-thawing circles. Here PVP was incorporated by linking with PVA to form a network structure, while the introduction of borax played the role of crosslinking PVA chains to accelerate the formation of a dual network structure in PVA/PVP composite hydrogel, thus endowing the hydrogel with high mechanical properties. The effects of both PVP and borax on the hydrogels were evaluated by comparing the two systems of PVA/PVP/borax and PVA/borax hydrogels. In the former system, adding 4.0% PVP not only increased the water content and the storage modulus but also enhanced the mechanical strength of the final hydrogel. But an overdose of PVP just as more than 4.0% tended to undermine the structure of hydrogels, and thus deteriorated hydrogels’ properties because of the weakened secondary interaction between PVP and PVA. Likewise, increasing borax could promote the gel crosslinking degree, thus making gels show a decrease in water content and swelling ratio, meanwhile shrinking the pores inside the hydrogels and finally enhancing the mechanical strength of hydrogels prominently. The developed hydrogel with high performances holds great potential for applications in biomedical and industrial fields. PMID:29491822

Functional nucleic acid-based hydrogels for bioanalytical and biomedical applications

PubMed Central

Mo, Liuting; Lu, Chun-Hua; Fu, Ting

2016-01-01

Hydrogels are crosslinked hydrophilic polymers that can absorb a large amount of water. By their hydrophilic, biocompatible and highly tunable nature, hydrogels can be tailored for applications in bioanalysis and biomedicine. Of particular interest are DNA-based hydrogels owing to the unique features of nucleic acids. Since the discovery of DNA double helical structure, interest in DNA has expanded beyond its genetic role to applications in nanotechnology and materials science. In particular, DNA-based hydrogels present such remarkable features as stability, flexibility, precise programmability, stimuli-responsive DNA conformations, facile synthesis and modification. Moreover, functional nucleic acids (FNAs) have allowed the construction of hydrogels based on aptamers, DNAzymes, i-motif nanostructures, siRNAs and CpG oligodeoxynucleotides to provide additional molecular recognition, catalytic activities and therapeutic potential, making them key players in biological analysis and biomedical applications. To date, a variety of applications have been demonstrated with FNA-based hydrogels, including biosensing, environmental analysis, controlled drug release, cell adhesion and targeted cancer therapy. In this review, we focus on advances in the development of FNA-based hydrogels, which have fully incorporated both the unique features of FNAs and DNA-based hydrogels. We first introduce different strategies for constructing DNA-based hydrogels. Subsequently, various types of FNAs and the most recent developments of FNA-based hydrogels for bioanalytical and biomedical applications are described with some selected examples. Finally, the review provides an insight into the remaining challenges and future perspectives of FNA-based hydrogels. PMID:26758955

Accelerated Leach Testing of GLASS (ALTGLASS): I. Informatics approach to high level waste glass gel formation and aging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jantzen, Carol M.; Trivelpiece, Cory L.; Crawford, Charles L.

Glass corrosion data from the ALTGLASS™ database were used to determine if gel compositions, which evolve as glass systems corrode, are correlated with the generation of zeolites and subsequent increase in the glass dissolution rate at long times. The gel compositions were estimated based on the difference between the elemental glass starting compositions and the measured elemental leachate concentrations from the long-term product consistency tests (ASTM C1285) at various stages of dissolution, ie, reaction progress. A well-characterized subset of high level waste glasses from the database was selected: these glasses had been leached for 15-20 years at reaction progresses upmore » to ~80%. The gel composition data, at various reaction progresses, were subjected to a step-wise regression, which demonstrated that hydrogel compositions with Si*/Al* ratios of <1.0 did not generate zeolites and maintained low dissolution rates for the duration of the experiments. Glasses that formed hydrogel compositions with Si^*/Al^* ratios ≥1, generated zeolites accompanied by a resumption in the glass dissolution rate. Finally, the role of the gel Si/Al ratio, and the interactions with the leachate, provides the fundamental understanding needed to predict if and when the glass dissolution rate will increase due to zeolitization.« less

Accelerated Leach Testing of GLASS (ALTGLASS): I. Informatics approach to high level waste glass gel formation and aging

DOE PAGES

Jantzen, Carol M.; Trivelpiece, Cory L.; Crawford, Charles L.; ...

2017-02-18

Glass corrosion data from the ALTGLASS™ database were used to determine if gel compositions, which evolve as glass systems corrode, are correlated with the generation of zeolites and subsequent increase in the glass dissolution rate at long times. The gel compositions were estimated based on the difference between the elemental glass starting compositions and the measured elemental leachate concentrations from the long-term product consistency tests (ASTM C1285) at various stages of dissolution, ie, reaction progress. A well-characterized subset of high level waste glasses from the database was selected: these glasses had been leached for 15-20 years at reaction progresses upmore » to ~80%. The gel composition data, at various reaction progresses, were subjected to a step-wise regression, which demonstrated that hydrogel compositions with Si*/Al* ratios of <1.0 did not generate zeolites and maintained low dissolution rates for the duration of the experiments. Glasses that formed hydrogel compositions with Si^*/Al^* ratios ≥1, generated zeolites accompanied by a resumption in the glass dissolution rate. Finally, the role of the gel Si/Al ratio, and the interactions with the leachate, provides the fundamental understanding needed to predict if and when the glass dissolution rate will increase due to zeolitization.« less

The bio in the ink: cartilage regeneration with bioprintable hydrogels and articular cartilage-derived progenitor cells.

PubMed

Levato, Riccardo; Webb, William R; Otto, Iris A; Mensinga, Anneloes; Zhang, Yadan; van Rijen, Mattie; van Weeren, René; Khan, Ilyas M; Malda, Jos

2017-10-01

Cell-laden hydrogels are the primary building blocks for bioprinting, and, also termed bioinks, are the foundations for creating structures that can potentially recapitulate the architecture of articular cartilage. To be functional, hydrogel constructs need to unlock the regenerative capacity of encapsulated cells. The recent identification of multipotent articular cartilage-resident chondroprogenitor cells (ACPCs), which share important traits with adult stem cells, represents a new opportunity for cartilage regeneration. However, little is known about the suitability of ACPCs for tissue engineering, especially in combination with biomaterials. This study aimed to investigate the potential of ACPCs in hydrogels for cartilage regeneration and biofabrication, and to evaluate their ability for zone-specific matrix production. Gelatin methacryloyl (gelMA)-based hydrogels were used to culture ACPCs, bone marrow mesenchymal stromal cells (MSCs) and chondrocytes, and as bioinks for printing. Our data shows ACPCs outperformed chondrocytes in terms of neo-cartilage production and unlike MSCs, ACPCs had the lowest gene expression levels of hypertrophy marker collagen type X, and the highest expression of PRG4, a key factor in joint lubrication. Co-cultures of the cell types in multi-compartment hydrogels allowed generating constructs with a layered distribution of collagens and glycosaminoglycans. By combining ACPC- and MSC-laden bioinks, a bioprinted model of articular cartilage was generated, consisting of defined superficial and deep regions, each with distinct cellular and extracellular matrix composition. Taken together, these results provide important information for the use of ACPC-laden hydrogels in regenerative medicine, and pave the way to the biofabrication of 3D constructs with multiple cell types for cartilage regeneration or in vitro tissue models. Despite its limited ability to repair, articular cartilage harbors an endogenous population of progenitor cells (ACPCs), that to date, received limited attention in biomaterials and tissue engineering applications. Harnessing the potential of these cells in 3D hydrogels can open new avenues for biomaterial-based regenerative therapies, especially with advanced biofabrication technologies (e.g. bioprinting). This study highlights the potential of ACPCs to generate neo-cartilage in a gelatin-based hydrogel and bioink. The ACPC-laden hydrogel is a suitable substrate for chondrogenesis and data shows it has a bias in directing cells towards a superficial zone phenotype. For the first time, ACPC-hydrogels are evaluated both as alternative for and in combination with chondrocytes and MSCs, using co-cultures and bioprinting for cartilage regeneration in vitro. This study provides important cues on ACPCs, indicating they represent a promising cell source for the next generation of cartilage constructs with increased biomimicry. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Hydrogels with a Memory: Dual-Responsive, Organometallic Poly(ionic liquid)s with Hysteretic Volume-Phase Transition

PubMed Central

2017-01-01

We report on the synthesis and structure–property relations of a novel, dual-responsive organometallic poly(ionic liquid) (PIL), consisting of a poly(ferrocenylsilane) backbone of alternating redox-active, silane-bridged ferrocene units and tetraalkylphosphonium sulfonate moieties in the side groups. This PIL is redox responsive due to the presence of ferrocene in the backbone and also exhibits a lower critical solution temperature (LCST)-type thermal responsive behavior. The LCST phase transition originates from the interaction between water molecules and the ionic substituents and shows a concentration-dependent, tunable transition temperature in aqueous solution. The PIL’s LCST-type transition temperature can also be influenced by varying the redox state of ferrocene in the polymer main chain. As the polymer can be readily cross-linked and is easily converted into hydrogels, it represents a new dual-responsive materials platform. Interestingly, the as-formed hydrogels display an unusual, strongly hysteretic volume-phase transition indicating useful thermal memory properties. By employing the dispersing abilities of this cationic PIL, CNT-hydrogel composites were successfully prepared. These hybrid conductive composite hydrogels showed bi-stable states and tunable resistance in heating–cooling cycles. PMID:28654756

Augmenting in vitro osteogenesis of a glycine-arginine-glycine-aspartic-conjugated oxidized alginate-gelatin-biphasic calcium phosphate hydrogel composite and in vivo bone biogenesis through stem cell delivery.

PubMed

Linh, Nguyen Tb; Paul, Kallyanashis; Kim, Boram; Lee, Byong-Taek

2016-11-01

A functionally modified peptide-conjugated hydrogel system was fabricated with oxidized alginate/gelatin loaded with biphasic calcium phosphate to improve its biocompatibility and functionality. Sodium alginate was treated by controlled oxidation to transform the cis-diol group into an aldehyde group in a controlled manner, which was then conjugated to the amine terminus of glycine-arginine-glycine-aspartic. Oxidized alginate glycine-arginine-glycine-aspartic was then combined with gelatin-loaded biphasic calcium phosphate to form a hydrogel of composite oxidized alginate/gelatin/biphasic calcium phosphate that displayed enhanced human adipose stem cell adhesion, spreading and differentiation. 1 H nuclear magnetic resonance and electron spectroscopy for chemical analysis confirmed that the glycine-arginine-glycine-aspartic was successfully grafted to the oxidized alginate. Co-delivery of glycine-arginine-glycine-aspartic and human adipose stem cell in a hydrogel matrix was studied with the results indicating that hydrogel incorporated modified with glycine-arginine-glycine-aspartic and seeded with human adipose stem cell enhanced osteogenesis in vitro and bone formation in vivo. © The Author(s) 2016.

Calcification capacity of porous pHEMA-TiO₂ composite hydrogels.

PubMed

Li, Chao; Zheng, Yu-Feng; Lou, Xia

2009-11-01

Many investigations have been attempted to promote calcification of synthetic polymers for applications as orthopaedic and dental implants. In this study, novel titanium dioxide (TiO(2)) reinforced porous poly(2-hydroxyethyl methacrylate) (pHEMA) hydrogels were synthesized. Calcification capacity of the composite polymers was examined using light microscopy, scanning electron microscopy and Fourier transform infrared spectroscopy after incubation of the materials in a simulated body fluid up to 53 days. Mechanical strength, porosity and in vitro cytotoxicity were also investigated. Calcification capacity of porous pHEMA was significantly enhanced by the addition of TiO(2) particulates. Infiltration of calcium phosphate, up to 1000 mum, was observed. The diffusion capacity of calcium ions was affected by the porosity and the interconnectivity of pores in the hydrogel polymers which were influenced by the presence of TiO(2) and the monomer concentration. Cell viability tests indicated that porous hydrogels containing 7.5% TiO(2) were not toxic to 3T3 fibroblast cells. These results demonstrate that incorporating TiO(2) nanoparticulates can promote enhanced formation of calcium phosphate whilst maintaining the porosity and interconnectivity of the hydrogel polymers and would be very useful for the development of orthopaedic tissue engineering scaffolds.

In vitro-ex vivo correlations between a cell-laden hydrogel and mucosal tissue for screening composite delivery systems.

PubMed

Blakney, Anna K; Little, Adam B; Jiang, Yonghou; Woodrow, Kim A

2016-11-01

Composite delivery systems where drugs are electrospun in different layers and vary the drug stacking-order are posited to affect bioavailability. We evaluated how the formulation characteristics of both burst- and sustained-release electrospun fibers containing three physicochemically diverse drugs: dapivirine (DPV), maraviroc (MVC) and tenofovir (TFV) affect in vitro and ex vivo release. We developed a poly(hydroxyethyl methacrylate) (pHEMA) hydrogel release platform for the rapid, inexpensive in vitro evaluation of burst- and sustained-release topical or dermal drug delivery systems with varying microarchitecture. We investigated properties of the hydrogel that could recapitulate ex vivo release into nonhuman primate vaginal tissue. Using a dimethyl sulfoxide extraction protocol and high-performance liquid chromatography analysis, we achieved >93% recovery from the hydrogels and >88% recovery from tissue explants for all three drugs. We found that DPV loading, but not stacking order (layers of fiber containing a single drug) or microarchitecture (layers with isolated drug compared to all drugs in the same layer) impacted the burst release in vitro and ex vivo. Our burst-release formulations showed a correlation for DPV accumulation between the hydrogel and tissue (R 2 =   0.80), but the correlation was not significant for MVC or TFV. For the sustained-release formulations, the PLGA/PCL content did not affect TFV release in vitro or ex vivo. Incorporation of cells into the hydrogel matrix improved the correlation between hydrogel and tissue explant release for TFV. We expect that this hydrogel-tissue mimic may be a promising preclinical model to evaluate topical or transdermal drug delivery systems with complex microarchitectures.

Lipogels responsive to near-infrared light for the triggered release of therapeutic agents.

PubMed

Martín-Saavedra, Francisco; Ruiz-Hernández, Eduardo; Escudero-Duch, Clara; Prieto, Martín; Arruebo, Manuel; Sadeghi, Negar; Deckers, Roel; Storm, Gert; Hennink, Wim E; Santamaría, Jesús; Vilaboa, Nuria

2017-10-01

Here we report a composite system based on fibrin hydrogels that incorporate in their structure near-infrared (NIR) responsive nanomaterials and thermosensitive liposomes (TSL). Polymerized fibrin networks entrap simultaneously gold-based nanoparticles (NPs) capable of transducing NIR photon energy into heat, and lysolipid-incorporated TSL (LTSL) loaded with doxorubicin hydrochloride (DOX). NIR irradiation of the resulting hydrogels (referred to as "lipogels") with 808nm laser light increased the temperature of the illuminated areas, leading to the release of the liposomal cargo. Levels of DOX that release from the "smart" composites were dependent on the concentration of NIR nanotransducers loaded in the lipogel, the intensity of the electromagnetic energy deposited and the irradiation regime. Released DOX retained its bioactivity, as shown in cultures of epithelial carcinoma cells. Finally, the developed drug delivery platform was refined by using NIR-photoabsorbers based on copper sulfide NPs to generate completely biodegradable composites as well as through the incorporation of cholesterol (Ch) in LTSL formulation, which lessens leakiness of the liposomal cargo at physiological temperature. This remotely controlled system may suit well for those therapies that require precise control over the dose of delivered drug in a defined spatiotemporal framework. Hydrogels composed of fibrin embedding nanoparticles responsive to near infrared (NIR) energy and thermosensitive liposomes loaded with doxorubicin hydrochloride (DOX), were prepared by in situ polymerization. NIR-light irradiation of these constructs, referred to as "NIR responsive lipogels", results in the controlled release of DOX to the surrounding medium. This technology may use fully degradable components and can preserve the bioactivity of liposomal cargo after remote triggering to finely regulate the dose and bioavailability of delivered payloads. NIR responsive lipogels technology overcomes the limitations of drug release systems based on the combination of liposomes and degradable polymeric materials, which in many cases lead to insufficient release at therapy onset or to overdose during high degradation period. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

GREAT-a randomized controlled trial comparing HydroSoft/HydroFrame and bare platinum coils for endovascular aneurysm treatment: procedural safety and core-lab-assessedangiographic results.

PubMed

Taschner, Christian A; Chapot, René; Costalat, Vincent; Machi, Paolo; Courthéoux, Patrick; Barreau, Xavier; Berge, Jérôme; Pierot, Laurent; Kadziolka, Kryzsztof; Jean, Betty; Blanc, Raphaël; Biondi, Alessandra; Brunel, Hervé; Gallas, Sophie; Berlis, Ansgar; Herbreteau, Denis; Berkefeld, Joachim; Urbach, Horst; El Shikh, Samer; Fiehler, Jens; Desal, Hubert; Graf, Erika; Bonafé, Alain

2016-08-01

Hybrid hydrogel-platinum coils (HydroCoil) have proven effective for endovascular aneurysm treatment. To overcome technical limitations (coil stiffness, time restriction for placement), a second generation of softer hydrogel coils has been brought to clinical practice (HydroSoft, HydroFrame). We report on procedural safety and core-lab-assessed angiographic results from an open-label multicenter randomized controlled trial. Web-based randomization occurred in 15 medical centers in France and seven in Germany between coil embolization with second-generation hydrogel coils and treatment with any bare platinum coil. Assist devices could be used as clinically required. Primary endpoint is a composite outcome including major aneurysm recurrence and poor clinical outcome at 18 months follow-up. Five hundred thirteen patients were randomized (hydrogel n = 256, bare platinum n = 257). Twenty patients were excluded for missing informed consent and nine patients for treatment related criteria. Four hundred eighty-four patients were analyzed as randomized (hydrogel n = 243, bare platinum n = 241). Two hundred eight had ruptured aneurysms (43 %). Prespecified procedural complications occurred in 58 subjects (hydrogel n = 28, bare platinum n = 30, p = 0.77). The 14-day mortality rate was 2.1 % in both arms of the study. The median calculated packing densities for aneurysms assigned to hydrogel and bare platinum were 39 and 31 % respectively (p < 0.001). No statistically significant differences were found between arms in the post procedural angiographic occlusion rate (p = 0.8). Second-generation hydrogel coils can be used in a wide spectrum of aneurysms with a risk profile equivalent to bare platinum. Packing density was significantly higher in aneurysms treated with hydrogel coils. http://www.germanctr.de , DRKS00003132.

Sustained prevention of biofilm formation on a novel silicone matrix suitable for medical devices.

PubMed

Steffensen, Søren Langer; Vestergaard, Merete Hedemark; Groenning, Minna; Alm, Martin; Franzyk, Henrik; Nielsen, Hanne Mørck

2015-08-01

Bacterial colonization and biofilm formation on medical devices constitute major challenges in clinical long-term use of e.g. catheters due to the risk of (re)infection of patients, which would result in additional use of antibiotics risking bacterial resistance development. The aim of the present project was to introduce a novel antibacterial approach involving an advanced composite material applicable for medical devices. The polymeric composites investigated consisted of a hydrogel network of cross-linked poly(2-hydroxyethyl methacrylate) (PHEMA) embedded in a poly(dimethylsiloxane) (PDMS) silicone elastomer produced using supercritical carbon dioxide (scCO2). In these materials, the hydrogel may contain an active pharmaceutical ingredient while the silicone elastomer provides the sufficient mechanical stability of the material. In these conceptual studies, the antimicrobial agent ciprofloxacin was loaded into the polymer matrix by a post-polymerization loading procedure. Sustained release of ciprofloxacin was demonstrated, and the release could be controlled by varying the hydrogel content in the range 13-38% (w/w) and by changing the concentration of ciprofloxacin during loading in the range of 1-20mg/mL. Devices containing 25% (w/w) hydrogel and loaded with ciprofloxacin displayed a strong antibacterial effect against Staphylococcus aureus bacterial colonization and subsequent biofilm formation on the device material was inhibited for 29days. In conclusion, the hydrogel/silicone composite represents a promising candidate material for medical devices that prevent bacterial colonization during long-term use. Copyright © 2015 Elsevier B.V. All rights reserved.

Cellulose fibers extracted from rice and oat husks and their application in hydrogel.

PubMed

Oliveira, Jean Paulo de; Bruni, Graziella Pinheiro; Lima, Karina Oliveira; Halal, Shanise Lisie Mello El; Rosa, Gabriela Silveira da; Dias, Alvaro Renato Guerra; Zavareze, Elessandra da Rosa

2017-04-15

The commercial cellulose fibers and cellulose fibers extracted from rice and oat husks were analyzed by chemical composition, morphology, functional groups, crystallinity and thermal properties. The cellulose fibers from rice and oat husks were used to produce hydrogels with poly (vinyl alcohol). The fibers presented different structural, crystallinity, and thermal properties, depending on the cellulose source. The hydrogel from rice cellulose fibers had a network structure with a similar agglomeration sponge, with more homogeneous pores compared to the hydrogel from oat cellulose fibers. The hydrogels prepared from the cellulose extracted from rice and oat husks showed water absorption capacity of 141.6-392.1% and high opacity. The highest water absorption capacity and maximum stress the compression were presented by rice cellulose hydrogel at 25°C. These results show that the use of agro-industrial residues is promising for the biomaterial field, especially in the preparation of hydrogels. Copyright © 2016 Elsevier Ltd. All rights reserved.

Influence of graphene-oxide nanosheets impregnation on properties of sterculia gum-polyacrylamide hydrogel formed by radiation induced polymerization.

PubMed

Singh, Baljit; Singh, Baldev

2017-06-01

Present work is an attempt, to explore the potential of graphene oxide nanoplates impregnation, on the mechanical and drug delivery properties of sterculia gum-polyacrylamide composite hydrogel formed by radiation induced polymerization. These polymers were characterized by SEM, cryo-SEM, AFM, FTIR's, 13 C NMR and swelling studies. Release profile of an anticancer drug 'gemcitabine' was studied to determine the drug release mechanism and best fit kinetic model. Furthermore, some important biomedical properties of the polymers such as blood compatibility, mucoadhesion, antioxidant properties and gel strength were also studied. Impregnation of GO into sterculia gum-poly(AAm) hydrogels decreased the swelling of hydrogels but improved the mechanical, drug loading and drug release properties of the hydrogels. Release of gemcitabine from drug loaded hydrogels occurred through non-Fickian diffusion mechanism and release profile was best fitted in first order kinetic model. These hydrogels have been found as haemocompatible, mucoadhesive, and antioxidant in nature. Copyright © 2017 Elsevier B.V. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perovic, Iva; Davidyants, Anastasia; Evans, John Spencer

In the mollusk shell there exists a framework silk fibroin-polysaccharide hydrogel coating around nacre aragonite tablets, and this coating facilitates the synthesis and organization of mineral nanoparticles into mesocrystals. In this report, we identify that a protein component of this coating, n16.3, is a hydrogelator. Due to the presence of intrinsic disorder, aggregation-prone regions, and nearly equal balance of anionic and cationic side chains, this protein assembles to form porous mesoscale hydrogel particles in solution and on mica surfaces. These hydrogel particles change their dimensionality, organization, and internal structure in response to pH and ions, particularly Ca(II), which indicates thatmore » these behave as ion-responsive or “smart” hydrogels. Thus, in addition to silk fibroins, the gel phase of the mollusk shell nacre framework layer may actually consist of several framework hydrogelator proteins, such as n16.3, which can promote mineral nanoparticle organization and assembly during the nacre biomineralization process and also serve as a model system for designing ion-responsive, composite, and smart hydrogels.« less

Development and Translation of a Tissue-Engineered Disc in a Preclinical Rodent Model

DTIC Science & Technology

2012-10-01

DAPS AF constructs, fabricated complete DAPS comprised of a PCL nanofiber AF and a hyaluronic acid hydrogel NP, and designed and commencement of...of a PCL nanofiber AF and a hyaluronic acid hydrogel NP, and design and commencement of construction of a novel multi-axis bioreactor that will be... nanofiber AF and a hyaluronic acid hydrogel NP We have commenced fabrication and in vitro pre-culture of composite DAPS constructs. An AF region

Aragonite-Associated Mollusk Shell Protein Aggregates To Form Mesoscale “Smart” Hydrogels

DOE PAGES

Perovic, Iva; Davidyants, Anastasia; Evans, John Spencer

2016-11-30

In the mollusk shell there exists a framework silk fibroin-polysaccharide hydrogel coating around nacre aragonite tablets, and this coating facilitates the synthesis and organization of mineral nanoparticles into mesocrystals. In this report, we identify that a protein component of this coating, n16.3, is a hydrogelator. Due to the presence of intrinsic disorder, aggregation-prone regions, and nearly equal balance of anionic and cationic side chains, this protein assembles to form porous mesoscale hydrogel particles in solution and on mica surfaces. These hydrogel particles change their dimensionality, organization, and internal structure in response to pH and ions, particularly Ca(II), which indicates thatmore » these behave as ion-responsive or “smart” hydrogels. Thus, in addition to silk fibroins, the gel phase of the mollusk shell nacre framework layer may actually consist of several framework hydrogelator proteins, such as n16.3, which can promote mineral nanoparticle organization and assembly during the nacre biomineralization process and also serve as a model system for designing ion-responsive, composite, and smart hydrogels.« less

Polymer-induced compression of biological hydrogels

NASA Astrophysics Data System (ADS)

Datta, Sujit; Preska Steinberg, Asher; Ismagilov, Rustem

Hydrogels - such as mucus, blood clots, and the extracellular matrix - provide critical functions in biological systems. However, little is known about how their structure is influenced by many of the polymeric materials they come into contact with regularly. Here, we focus on one critically important biological hydrogel: colonic mucus. While several biological processes are thought to potentially regulate the mucus hydrogel structure, the polymeric composition of the gut environment has been ignored. We use Flory-Huggins solution theory to characterize polymer-mucus interactions. We find that gut polymers, including those small enough to penetrate the mucus hydrogel, can in fact alter mucus structure, changing its equilibrium degree of swelling and forcing it to compress. The extent of compression increases with increasing polymer concentration and size. We use experiments on mice to verify these predictions with common dietary and therapeutic gut polymers. Our results provide a foundation for investigating similar, previously overlooked, polymer-induced effects in other biological hydrogels.

Design and fabrication of a chitosan hydrogel with gradient structures via a step-by-step cross-linking process.

PubMed

Xu, Yongxiang; Yuan, Shenpo; Han, Jianmin; Lin, Hong; Zhang, Xuehui

2017-11-15

The development of scaffolds to mimic the gradient structure of natural tissue is an important consideration for effective tissue engineering. In the present study, a physical cross-linking chitosan hydrogel with gradient structures was fabricated via a step-by-step cross-linking process using sodium tripolyphosphate and sodium hydroxide as sequential cross-linkers. Chitosan hydrogels with different structures (single, double, and triple layers) were prepared by modifying the gelling process. The properties of the hydrogels were further adjusted by varying the gelling conditions, such as gelling time, pH, and composition of the crosslinking solution. Slight cytotoxicity was showed in MTT assay for hydrogels with uncross-linking chitosan solution and non-cytotoxicity was showed for other hydrogels. The results suggest that step-by-step cross-linking represents a practicable method to fabricate scaffolds with gradient structures. Copyright © 2017. Published by Elsevier Ltd.

Genipin-crosslinked gelatin-silk fibroin hydrogels for modulating the behaviour of pluripotent cells.

PubMed

Sun, Wei; Incitti, Tania; Migliaresi, Claudio; Quattrone, Alessandro; Casarosa, Simona; Motta, Antonella

2016-10-01

Different hydrogel materials have been prepared to investigate the effects of culture substrate on the behaviour of pluripotent cells. In particular, genipin-crosslinked gelatin-silk fibroin hydrogels of different compositions have been prepared, physically characterized and used as substrates for the culture of pluripotent cells. Pluripotent cells cultured on hydrogels remained viable and proliferated. Gelatin and silk fibroin promoted the proliferation of cells in the short and long term, respectively. Moreover, cells cultured on genipin-crosslinked gelatin-silk fibroin blended hydrogels were induced to an epithelial ectodermal differentiation fate, instead of the neural ectodermal fate obtained by culturing on tissue culture plates. This work confirms that specific culture substrates can be used to modulate the behaviour of pluripotent cells and that our genipin-crosslinked gelatin-silk fibroin blended hydrogels can induce pluripotent cells differentiation to an epithelial ectodermal fate. Copyright © 2014 John Wiley & Sons, Ltd. Copyright © 2014 John Wiley & Sons, Ltd.

Stimuli-sensitive hydrogels: an excellent carrier for drug and cell delivery.

PubMed

Garg, Tarun; Singh, Simranjit; Goyal, Amit Kumar

2013-01-01

The stimuli-sensitive hydrogel is an injectable formulation that is used to deliver drugs, cells, and genes into the body. Hydrogels are available in various physical forms such as solid molded, pressed powder matrix, microparticle, coating, or membrane forms. The network structure of hydrogels can be macroporous, microporous, or nonporous. Different categories of biomaterials, such as natural, synthetic, and combinations (e.g., semisynthetic such as natural-natural, natural-synthetic, and synthetic-synthetic polymers), are commonly used in hydrogel preparation. Classification of hydrogels mainly depends upon physical stimuli (temperature, electric fields, solvent composition, light, pressure, sound, and magnetic fields) and chemical or biochemical stimuli (pH, ions, and specific molecular recognition events). Several approaches for the synthesis of hydrogels have been reported, including emulsification, micromolding, photolithography, isostatic ultra high pressure, and microfluidic techniques. Hydrogels provide structural integrity and cellular organization, serve as tissue barriers, act as bioadhesive and drug depots, deliver bioactive agents and cells, and possess unique swelling properties and structures. This review provides a detailed account of the need for development of hydrogels, along with the materials used and techniques adopted to manufacture scaffolds for tissue engineering and for prolonged drug, cell, and gene delivery.

Application of Hydrogels in Heart Valve Tissue Engineering

PubMed Central

Zhang, Xing; Xu, Bin; Puperi, Daniel S.; Wu, Yan; West, Jennifer L.; Grande-Allen, K. Jane

2015-01-01

With an increasing number of patients requiring valve replacement, there is heightened interest in advancing heart valve tissue engineering (HVTE) to provide solutions to the many limitations of current surgical treatments. A variety of materials have been developed as scaffolds for HVTE including natural polymers, synthetic polymers, and decellularized valvular matrices. Among them, biocompatible hydrogels are generating growing interest. Natural hydrogels, such as collagen and fibrin, generally show good bioactivity, but poor mechanical durability. Synthetic hydrogels, on the other hand, have tunable mechanical properties; however, appropriate cell-matrix interactions are difficult to obtain. Moreover, hydrogels can be used as cell carriers when the cellular component is seeded into the polymer meshes or decellularized valve scaffolds. In this review, we discuss current research strategies for HVTE with an emphasis on hydrogel applications. The physicochemical properties and fabrication methods of these hydrogels, as well as their mechanical properties and bioactivities are described. Performance of some hydrogels including in vitro evaluation using bioreactors and in vivo tests in different animal models are also discussed. For future HVTE, it will be compelling to examine how hydrogels can be constructed from composite materials to replicate mechanical properties and mimic biological functions of the native heart valve. PMID:25955010

Structure and mechanical properties of supramolecular random copolymer hydrogels cross linked by hydrophobic aggregates.

NASA Astrophysics Data System (ADS)

Vogt, Bryan; Wiener, Clinton; Wang, Chao; Weiss, Bob

Stress dissipation mechanisms are critical to improving the toughness of hydrogels. The use of reversible hydrophobic associations for crosslnking of hydrogels provides such a mechanism for toughening, but can also lead to the creep of the hydrogel as the crosslinks break and reform. The morphology of the hydrophobic aggregates thus is critical to the mechanical properties of the hydrogels. In this work, we will demonstrate how the processing of these copolymers impacts the hydrogel structure and this structure is correlated with the mechanical properties through a combination of small angle scattering, rheology, and tensile measurements. The hydrophilic and hydrophobic chemistries in the copolymer can be used to tune the water content and strength of the crosslinks, while the copolymer composition provides the number density of crosslinks and also acts to modulate the swelling of the hydrogel. These copolymers as well as their hydrogels can in general use traditional polymer processing, but the details of this processing impacts both the nanoscale morphology and the resultant mechanical properties of the hydrogels. This work was financially supported by the Civil, Mechanical and Manufacturing Innovation (CMMI) Division in the Directorate for Engineering of the National Science Foundation, Grant. CMMI-1300212.

Injectable Hydrogels for Cardiac Tissue Repair after Myocardial Infarction

PubMed Central

Khattab, Ahmad; Islam, Mohammad Ariful; Hweij, Khaled Abou; Zeitouny, Joya; Waters, Renae; Sayegh, Malek; Hossain, Md Monowar; Paul, Arghya

2015-01-01

Cardiac tissue damage due to myocardial infarction (MI) is one of the leading causes of mortality worldwide. The available treatments of MI include pharmaceutical therapy, medical device implants, and organ transplants, all of which have severe limitations including high invasiveness, scarcity of donor organs, thrombosis or stenosis of devices, immune rejection, and prolonged hospitalization time. Injectable hydrogels have emerged as a promising solution for in situ cardiac tissue repair in infarcted hearts after MI. In this review, an overview of various natural and synthetic hydrogels for potential application as injectable hydrogels in cardiac tissue repair and regeneration is presented. The review starts with brief discussions about the pathology of MI, its current clinical treatments and their limitations, and the emergence of injectable hydrogels as a potential solution for post MI cardiac regeneration. It then summarizes various hydrogels, their compositions, structures and properties for potential application in post MI cardiac repair, and recent advancements in the application of injectable hydrogels in treatment of MI. Finally, the current challenges associated with the clinical application of injectable hydrogels to MI and their potential solutions are discussed to help guide the future research on injectable hydrogels for translational therapeutic applications in regeneration of cardiac tissue after MI. PMID:27668147

Mixed-Matrix Membranes Containing Carbon Nanotubes Composite with Hydrogel for Efficient CO2 Separation.

PubMed

Zhang, Haiyang; Guo, Ruili; Hou, Jinpeng; Wei, Zhong; Li, Xueqin

2016-10-26

In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO 2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO 2 transport through membranes, increasing CO 2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO 2 permeability and CO 2 /gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO 2 permeability of 567 barrer, CO 2 /CH 4 selectivity of 35, and CO 2 /N 2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO 2 separation performance of MMMs is mainly attributed to the construction of the efficient CO 2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO 2 separation.

Microplasma-assisted hydrogel fabrication: A novel method for gelatin-graphene oxide nano composite hydrogel synthesis for biomedical application

PubMed Central

2017-01-01

Toxicity issues and biocompatibility concerns with traditional classical chemical cross-linking processes prevent them from being universal approaches for hydrogel fabrication for tissue engineering. Physical cross-linking methods are non-toxic and widely used to obtain cross-linked polymers in a tunable manner. Therefore, in the current study, argon micro-plasma was introduced as a neutral energy source for cross-linking in fabrication of the desired gelatin-graphene oxide (gel-GO) nanocomposite hydrogel scaffolds. Argon microplasma was used to treat purified gelatin (8% w/v) containing 0.1∼1 wt% of high-functionality nano-graphene oxide (GO). Optimized plasma conditions (2,500 V and 8.7 mA) for 15 min with a gas flow rate of 100 standard cm3/min was found to be most suitable for producing the gel-GO nanocomposite hydrogels. The developed hydrogel was characterized by the degree of cross-linking, FTIR spectroscopy, SEM, confocal microscopy, swelling behavior, contact angle measurement, and rheology. The cell viability was examined by an MTT assay and a live/dead assay. The pore size of the hydrogel was found to be 287 ± 27 µm with a contact angle of 78° ± 3.7°. Rheological data revealed improved storage as well as a loss modulus of up to 50% with tunable viscoelasticity, gel strength, and mechanical properties at 37 °C temperature in the microplasma-treated groups. The swelling behavior demonstrated a better water-holding capacity of the gel-GO hydrogels for cell growth and proliferation. Results of the MTT assay, microscopy, and live/dead assay exhibited better cell viability at 1% (w/w) of high-functionality GO in gelatin. The highlight of the present study is the first successful attempt of microplasma-assisted gelatin-GO nano composite hydrogel fabrication that offers great promise and optimism for further biomedical tissue engineering applications. PMID:28663938

Nanocomposite particles with improved microstructure for 3D culture systems and bone regeneration.

PubMed

Cecoltan, Sergiu; Stancu, Izabela-Cristina; Drăguşin, Diana Maria; Serafim, Andrada; Lungu, Adriana; Ţucureanu, Cătălin; Caraş, Iuliana; Tofan, Vlad Constantin; Sălăgeanu, Aurora; Vasile, Eugeniu; Mallet, Romain; Chappard, Daniel; Coman, Cristin; Istodorescu, Mircea; Iovu, Horia

2017-08-31

Nano-apatite and gelatin-alginate hydrogel microparticles have been prepared by a one-step synthesis combined with electrostatic bead generation, for the reconstruction of bone defects. Based on the analysis of bone composition, architecture and embryonic intramembranous ossification, a bio-inspired fabrication has been developed. Accordingly, the mineral phase has been in situ synthesized, calcifying the hydrogel matrix while the latter was crosslinked, finally generating microparticles that can assemble into a bone defect to ensure interconnected pores. Although nano-apatite-biopolymer composites have been widely investigated, microstructural optimization to provide improved distribution and stability of the mineral is rarely achieved. The optimization of the developed method progressively resulted in two types of formulations (15P and 7.5P), with 15 and 7.5 (wt%) phosphate content in the initial precursor. The osteolytic potential was investigated using differentiated macrophages. A commercially available calcium phosphate bone graft substitute (Eurocer 400) was incorporated into the hydrogel, and the obtained composites were in vitro tested for comparison. The cytocompatibility of the microparticles was studied with mouse osteoblast-like cell line MC3T3-E1. Results indicated the best in vitro performance have been obtained for the sample loaded with 7.5P. Preliminary evaluation of biocompatibility into a critical size (3 mm) defect in rabbits showed that 7.5P nanocomposite is associated with newly formed bone in the proximity of the microparticles, after 28 days.

Chemically Crosslinked Hydrogel Film Leads to Integrated Flexible Supercapacitors with Superior Performance.

PubMed

Wang, Kai; Zhang, Xiong; Li, Chen; Sun, Xianzhong; Meng, Qinghai; Ma, Yanwei; Wei, Zhixiang

2015-12-02

A high-strength poly(vinyl alcohol) chemical hydrogel (PCH) film is prepared by coupling covalent crosslinking with a film-casting process. Conducting polyaniline (PANI) is then embedded in the PCH film by in situ growth to form a composite film with a PANI-hydrogel-PANI configuration, which leads to a new conceptual flexible supercapacitor with all-in-one configuration that exhibits superior electrochemical performance and mechanical flexibility. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Development and Translation of a Tissue-Engineered Disc in a Preclinical Rodent Model

DTIC Science & Technology

2012-10-29

PCL nanofiber AF and a hyaluronic acid hydrogel NP, and designed and commencement of construction of a multi-axis bioreactor that will be used to...of a PCL nanofiber AF and a hyaluronic acid hydrogel NP, and design and commencement of construction of a novel multi-axis bioreactor that will be... nanofiber AF and a hyaluronic acid hydrogel NP We have commenced fabrication and in vitro pre-culture of composite DAPS constructs. An AF region

Graphene hydrogels deposited in nickel foams for high-rate electrochemical capacitors.

PubMed

Chen, Ji; Sheng, Kaixuan; Luo, Peihui; Li, Chun; Shi, Gaoquan

2012-08-28

Graphene hydrogel/nickel foam composite electrodes for high-rate electrochemical capacitors are produced by reduction of an aqueous dispersion of graphene oxide in a nickel foam (upper half of figure). The micropores of the hydrogel are exposed to the electrolyte so that ions can enter and form electrochemical double-layers. The nickel framework shortens the distances of charge transfer. Therefore, the electrochemical capacitor exhibits highrate performance (see plots). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Degradable Bone Graft Substitute for Effective Delivery of Multiple Growth Factors in the Treatment of Nonunion Fractures

DTIC Science & Technology

2012-08-01

growth factors directly to the bone defect site can enhance repair of non-union fractures. In this study, a new chitosan /xylan composite hydrogel was...delivery aspect of this study did not succeed, treatment with the new xylan/ chitosan hydrogel alone was enough to heal serious fractures that did not...characteristics of the hydrogel in question could be tested as well as performing in vitro cell work. The previous supplier of chitosan , the main polymer

The effect of methylcellulose on metronidazole release from polyacrylic acid hydrogels.

PubMed

Musial, Witold

2007-08-01

Topical treatment of acne rosacea, a chronic condition characterized by recurrent course for many years, is primarily based on metronidazole preparations. The aim of this study was to evaluate the effect of various acrylic acid polymers, in composition with methylcellulose on metronidazole release rate from hydrogels proposed for the treatment of acne rosacea. Viscosity and release studies using "Paddle over Disk" system with semipermeable membrane of MWCO 3500 were performed. Compositions of Carbopol 971P and methylcellulose revealed an increase in viscosity with increasing concentration of methylcellulose in the range of 17200-26166 mPa.s. In all the examined formulations, the release process was characterized by a two-stage course. Among bipolymeric formulations, the highest first-stage release rate of 9.18 x 10(-3) min(-1) was determined for the gel consisting of 2.00% Carbopol 980NF with 1.00% methylcellulose. The second-stage release rates ranged between 2.88 x 10(-3) and 8.00 x 10(-3) min(-1). Two-stage release course can thus be attributed to metronidazole distribution into two compartments of hydrogel matrix. Proposed gels, with similar rheological properties, may be used for ex vivo and in vivo studies to obtain a suitable drug activity of metronidazole in the treatment of acne rosacea.

Physicochemical characteristics of Fe3O4 magnetic nanocomposites based on Poly(N-isopropylacrylamide) for anti-cancer drug delivery.

PubMed

Davaran, Soodabeh; Alimirzalu, Samira; Nejati-Koshki, Kazem; Nasrabadi, Hamid Tayef; Akbarzadeh, Abolfazl; Khandaghi, Amir Ahmad; Abbasian, Mojtaba; Alimohammadi, Somayeh

2014-01-01

Hydrogels are a class of polymers that can absorb water or biological fluids and swell to several times their dry volume, dependent on changes in the external environment. In recent years, hydrogels and hydrogel nanocomposites have found a variety of biomedical applications, including drug delivery and cancer treatment. The incorporation of nanoparticulates into a hydrogel matrix can result in unique material characteristics such as enhanced mechanical properties, swelling response, and capability of remote controlled actuation. In this work, synthesis of hydrogel nanocomposites containing magnetic nanoparticles are studied. At first, magnetic nanoparticles (Fe3O4) with an average size 10 nm were prepared. At second approach, thermo and pH-sensitive poly (N-isopropylacrylamide -co-methacrylic acid-co-vinyl pyrrolidone) (NIPAAm-MAA- VP) were prepared. Swelling behavior of co-polymer was studied in buffer solutions with different pH values (pH=5.8, pH=7.4) at 37 °C. Magnetic iron oxide nanoparticles (Fe3O4) and doxorubicin were incorporated into copolymer and drug loading was studied. The release of drug, carried out at different pH and temperatures. Finally, chemical composition, magnetic properties and morphology of doxorubicin-loaded magnetic hydrogel nanocomposites were analyzed by FT- IR, vibrating sample magnetometry (VSM), scanning electron microscopy (SEM). The results indicated that drug loading efficiency was increased by increasing the drug ratio to polymer. Doxorubicin was released more at 40 °C and in acidic pH compared to that 37 °C and basic pH. This study suggested that the poly (NIPAAm-MAA-VP) magnetic hydrogel nanocomposite could be an effective carrier for targeting drug delivery systems of anti-cancer drugs due to its temperature sensitive properties.

Optically- and Thermally-Responsive Programmable Materials Based on Carbon Nanotube-Hydrogel Polymer Composites

DTIC Science & Technology

2011-07-07

Jamshidi, Kuniharu Takei, Hyunhyub Ko, Andrew Gillies, Rizia Bardhan , Xiaobo Zhang, Jeffrey J. Urban, Ming Wu, Ali Javey, Ronald Fearing, Cary L...Hyunhyub Ko,†,‡,§ Andrew Gillies,† Rizia Bardhan ,|| Jeffrey J. Urban,|| Ming Wu,†,‡ Ronald Fearing,† and Ali Javey*,†,‡,§ †Electrical

Fabrications and Applications of Stimulus-Responsive Polymer Films and Patterns on Surfaces: A Review

PubMed Central

Chen, Jem-Kun; Chang, Chi-Jung

2014-01-01

In the past two decades, we have witnessed significant progress in developing high performance stimuli-responsive polymeric materials. This review focuses on recent developments in the preparation and application of patterned stimuli-responsive polymers, including thermoresponsive layers, pH/ionic-responsive hydrogels, photo-responsive film, magnetically-responsive composites, electroactive composites, and solvent-responsive composites. Many important new applications for stimuli-responsive polymers lie in the field of nano- and micro-fabrication, where stimuli-responsive polymers are being established as important manipulation tools. Some techniques have been developed to selectively position organic molecules and then to obtain well-defined patterned substrates at the micrometer or submicrometer scale. Methods for patterning of stimuli-responsive hydrogels, including photolithography, electron beam lithography, scanning probe writing, and printing techniques (microcontact printing, ink-jet printing) were surveyed. We also surveyed the applications of nanostructured stimuli-responsive hydrogels, such as biotechnology (biological interfaces and purification of biomacromoles), switchable wettability, sensors (optical sensors, biosensors, chemical sensors), and actuators. PMID:28788489

Cellulose gum and copper nanoparticles based hydrogel as antimicrobial agents against urinary tract infection (UTI) pathogens.

PubMed

Al-Enizi, Abdullah M; Ahamad, Tansir; Al-Hajji, Abdullah Baker; Ahmed, Jahangeer; Chaudhary, Anis Ahmad; Alshehri, Saad M

2018-04-01

In the present study, stable copper nanoparticles (CuNPs) were successfully prepared in the hydrogel matrix. The prepared nanocomposite (HCuNPs) was characterized via x-ray diffraction (XRD), electron microscopy (TEM), and energy-dispersive (EDX) and x-ray photoelectron spectroscopic (XPS) studies. The wide scan XPS spectra support the presence of C, N and O in neat hydrogel; while, the XPS spectra of HCuNPs demonstrate the presence of Cu along with C, N, and O elements. TEM studies show the formation of spherical shaped CuNPs in the size range from 7 to 12nm. The rheology results reveal that the storage modulus (G') of the HCuNPs was found to be higher than the loss modulus (G"). Additionally, the antibacterial activities and cytotoxic were carried out against urinary tract infection (UTI) microbes and HeLa (cervical) cells respectively. The antibacterial results reveal that HCuNPs composites show higher zone of inhibition against these pathogens then that of corresponding hydrogel matrix. The cytotoxic effects suggest that the prepared nanocomposite could be used as promising candidates for biomedical applications. Copyright © 2017 Elsevier B.V. All rights reserved.

Sterilization of silicone-based hydrogels for biomedical application using ozone gas: Comparison with conventional techniques.

PubMed

Galante, Raquel; Ghisleni, Daniela; Paradiso, Patrizia; Alves, Vitor D; Pinto, Terezinha J A; Colaço, Rogério; Serro, Ana Paula

2017-09-01

Sterilization of hydrogels is challenging due to their often reported sensitivity to conventional methods involving heat or radiation. Although aseptic manufacturing is a possibility, terminal sterilization is safer in biological terms, leading to a higher overall efficiency, and thus should be used whenever it is possible. The main goal of this work was to study the applicability of an innovative ozone gas terminal sterilization method for silicone-based hydrogels and compare its efficacy and effects with those of traditional sterilization methods: steam heat and gamma irradiation. Ozone gas sterilization is a method with potential interest since it is reported as a low cost green method, does not leave toxic residues and can be applied to thermosensitive materials. A hydrogel intended for ophthalmological applications, based on tris(trimethylsiloxy)silyl] propyl methacrylate, was prepared and extensively characterized before and after the sterilization procedures. Alterations regarding transparency, swelling, wettability, ionic permeability, friction coefficient, mechanical properties, topography and morphology and chemical composition were monitored. Efficacy of the ozonation was accessed by performing controlled contaminations and sterility tests. In vitro cytotoxicity testes were also performed. The results show that ozonation may be applied to sterilize the studied material. A treatment with 8 pulses allowed sterilizing the material with bioburdens≤10 3 CFU/mL, preserving all the studied properties within the required known values for contact lenses materials. However, a higher exposure (10 pulses) led to some degradation of the material and induced mild cytotoxicity. Steam heat sterilization led to an increase of swelling capacity and a decrease of the water contact angle. Regarding gamma irradiation, the increase of irradiation dose led to an increase of the friction coefficient. The higher dose (25kGy) originated surface degradation and affected the mechanical properties of the hydrogel by inducing a significant increase of the Young's modulus. Overall, the results show that ozonation may be considered as a valid and promising alternative for the sterilization of silicon-based hydrogels for biomedical applications. Copyright © 2017 Elsevier B.V. All rights reserved.

Flexible pH-Sensing Hydrogel Fibers for Epidermal Applications.

PubMed

Tamayol, Ali; Akbari, Mohsen; Zilberman, Yael; Comotto, Mattia; Lesha, Emal; Serex, Ludovic; Bagherifard, Sara; Chen, Yu; Fu, Guoqing; Ameri, Shideh Kabiri; Ruan, Weitong; Miller, Eric L; Dokmeci, Mehmet R; Sonkusale, Sameer; Khademhosseini, Ali

2016-03-01

Epidermal pH is an indication of the skin's physiological condition. For example, pH of wound can be correlated to angiogenesis, protease activity, bacterial infection, etc. Chronic nonhealing wounds are known to have an elevated alkaline environment, while healing process occurs more readily in an acidic environment. Thus, dermal patches capable of continuous pH measurement can be used as point-of-care systems for monitoring skin disorder and the wound healing process. Here, pH-responsive hydrogel fibers are presented that can be used for long-term monitoring of epidermal wound condition. pH-responsive dyes are loaded into mesoporous microparticles and incorporated into hydrogel fibers using a microfluidic spinning system. The fabricated pH-responsive microfibers are flexible and can create conformal contact with skin. The response of pH-sensitive fibers with different compositions and thicknesses are characterized. The suggested technique is scalable and can be used to fabricate hydrogel-based wound dressings with clinically relevant dimensions. Images of the pH-sensing fibers during real-time pH measurement can be captured with a smart phone camera for convenient readout on-site. Through image processing, a quantitative pH map of the hydrogel fibers and the underlying tissue can be extracted. The developed skin dressing can act as a point-of-care device for monitoring the wound healing process. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Prevascularization of 3D printed bone scaffolds by bioactive hydrogels and cell co-culture.

PubMed

Kuss, Mitchell A; Wu, Shaohua; Wang, Ying; Untrauer, Jason B; Li, Wenlong; Lim, Jung Yul; Duan, Bin

2017-09-13

Vascularization is a fundamental prerequisite for large bone construct development and remains one of the main challenges of bone tissue engineering. Our current study presents the combination of 3D printing technique with a hydrogel-based prevascularization strategy to generate prevascularized bone constructs. Human adipose derived mesenchymal stem cells (ADMSC) and human umbilical vein endothelial cells (HUVEC) were encapsulated within our bioactive hydrogels, and the effects of culture conditions on in vitro vascularization were determined. We further generated composite constructs by forming 3D printed polycaprolactone/hydroxyapatite scaffolds coated with cell-laden hydrogels and determined how the co-culture affected vascularization and osteogenesis. It was demonstrated that 3D co-cultured ADMSC-HUVEC generated capillary-like networks within the porous 3D printed scaffold. The co-culture systems promoted in vitro vascularization, but had no significant effects on osteogenesis. The prevascularized constructs were subcutaneously implanted into nude mice to evaluate the in vivo vascularization capacity and the functionality of engineered vessels. The hydrogel systems facilitated microvessel and lumen formation and promoted anastomosis of vascular networks of human origin with host murine vasculature. These findings demonstrate the potential of prevascularized 3D printed scaffolds with anatomical shape for the healing of larger bone defects. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 2017. © 2017 Wiley Periodicals, Inc.

Bioreactor mechanically guided 3D mesenchymal stem cell chondrogenesis using a biocompatible novel thermo-reversible methylcellulose-based hydrogel

PubMed Central

Cochis, A.; Grad, S.; Stoddart, M. J.; Farè, S.; Altomare, L.; Azzimonti, B.; Alini, M.; Rimondini, L.

2017-01-01

Autologous chondrocyte implantation for cartilage repair represents a challenge because strongly limited by chondrocytes’ poor expansion capacity in vitro. Mesenchymal stem cells (MSCs) can differentiate into chondrocytes, while mechanical loading has been proposed as alternative strategy to induce chondrogenesis excluding the use of exogenous factors. Moreover, MSC supporting material selection is fundamental to allow for an active interaction with cells. Here, we tested a novel thermo-reversible hydrogel composed of 8% w/v methylcellulose (MC) in a 0.05 M Na2SO4 solution. MC hydrogel was obtained by dispersion technique and its thermo-reversibility, mechanical properties, degradation and swelling were investigated, demonstrating a solution-gelation transition between 34 and 37 °C and a low bulk degradation (<20%) after 1 month. The lack of any hydrogel-derived immunoreaction was demonstrated in vivo by mice subcutaneous implantation. To induce in vitro chondrogenesis, MSCs were seeded into MC solution retained within a porous polyurethane (PU) matrix. PU-MC composites were subjected to a combination of compression and shear forces for 21 days in a custom made bioreactor. Mechanical stimulation led to a significant increase in chondrogenic gene expression, while histological analysis detected sulphated glycosaminoglycans and collagen II only in loaded specimens, confirming MC hydrogel suitability to support load induced MSCs chondrogenesis. PMID:28332587

The use of poly(vinyl phosphonic acid) microgels for the preparation of inherently magnetic Co metal catalyst particles in hydrogen production

NASA Astrophysics Data System (ADS)

Sahiner, Nurettin; Sagbas, Selin

2014-01-01

Novel poly(vinyl phosphonic acid) (p(VPA)) micro particle and composite p(VPA)-silica micro particle hydrogels are synthesized using a micro-emulsion polymerization technique. Porous p(VPA) particles are generated after removal of silica particles upon treatment of composite p(VPA) with 0.5 M NaOH solution. Bare, composite with silica, and porous p(VPA) micro particle hydrogels are used as templates and as reactors. Metal nanoparticles, Co, Ni, and Cu are generated in situ inside these hydrogels by chemical reduction of the absorbed metal ions with a reducing agent such as sodium boron hydride (NaBH4), and are used as catalyst in hydrogen production by hydrolysis of NaBH4 in a basic medium and ammonia borane (AB). The effects of reloaded metal ions, the reaction temperature, the porosity, the reusability, and the type of metal (Co, Ni, Cu) are investigated. The activation energy for hydrolysis of NaBH4, and AB by p(VPA)-Co is 28.02 and 25.51 kJ mol-1, respectively. The mass susceptibility measurements of composite p(VPA)-Co microgel is found as ferromagnetic. It is found that p(VPA) microgels provided better catalytic performance in comparison to macro p(VPA) hydrogels due to improved properties such as higher surface area, pore structure, and inherently magnetic behavior after multiple loadings-reduction of Co(II) from aqueous medium.

Hydrogel Biomaterials: A Smart Future?

PubMed Central

Kopeček, Jindřich

2007-01-01

Hydrogels were the first biomaterials developed for human use. The state-of-the-art and potential for the future are discussed. Recently, new designs have produced mechanically strong synthetic hydrogels. Protein based hydrogels and hybrid hydrogels containing protein domains present a novel advance; such biomaterials may self-assemble from block or graft copolymers containing biorecognition domains. One of the domains, the coiled-coil, ubiquitously found in nature, has been used as an example to demonstrate the developments in the design of smart hydrogels. The application potential of synthetic, protein-based, DNA-based, and hybrid hydrogels bodes well for the future of this class of biomaterials. PMID:17697712

Preparation of morphology-controllable polyaniline and polyaniline/graphene hydrogels for high performance binder-free supercapacitor electrodes

NASA Astrophysics Data System (ADS)

Luo, Jinwei; Zhong, Wenbin; Zou, Yubo; Xiong, Changlun; Yang, Wantai

2016-07-01

Polyaniline (PANI) and its composite hydrogels have been considered as a unique supercapacitor electrode material due to their three dimensional (3D) porous structures, formed conducting networks, high specific surface areas and fast electron/ion transfer. Herein, dendritic and long fibrous PANI nanostructure hydrogels (PDH and PFH), dendritic PNAI nanofiber/graphene and long PANI nanofibers/Nitrogen-doped graphene composite hydrogels (PGH and PNGH) were prepared by integration polymerization of aniline and hydrothermal process. It was found that the addition of p-Phenylenediamine (PPD) not only controlled the morphologies of PANI from dendritic to long fibrous, but also facilitated the graphene oxide (GO) into nitrogen-doped graphene. Furthermore, after freeze-drying, PDH and PGH exhibited a max compressive strength of 9.5 and 9.6 KPa, respectively; while the max compressive strength of PFH and PNGH constructed with long PANI nanofiber is 79.9 and 75.8 KPa, respectively. Directly using these prepared hydrogels as electrodes for supercapacitors, it was found that PDH, PFH, PGH and PNGH exhibited high specific capacitances of 448.6, 470, 540.9 and 610 F g-1, respectively, at the current density of 1 A g-1. It is expected that the prepared PDH, PFH, PGH and PNGH can be directly applied in the field of high performance energy storage devices.

Electromechanical response of silk fibroin hydrogel and conductive polycarbazole/silk fibroin hydrogel composites as actuator material.

PubMed

Srisawasdi, Thanida; Petcharoen, Karat; Sirivat, Anuvat; Jamieson, Alexander M

2015-11-01

Pure silk fibroin (SF) hydrogel and polycarbazole/silk fibroin (SF/PCZ) hydrogels were fabricated by solvent casting technique to evaluate electromechanical responses, dielectric properties, and cantilever deflection properties as functions of electric field strength, SF concentration, glutaraldehyde concentration, and PCZ concentration in the blends. Electromechanical properties were characterized in oscillatory shear mode at electric field strengths ranging from 0 to 600V/mm and at a temperature of 27°C. For both the pristine SF and SF/PCZ hydrogels, the storage modulus response (ΔG') and the storage modulus sensitivity (ΔG'/G'0) increased dramatically with increasing electric field strength. The pristine hydrogel possessed the highest storage modulus sensitivity value of 5.87, a relatively high value when compared with other previously studied electroactive polymers. With the addition of conductive PCZ in SF hydrogel, the storage modulus sensitivity and the relative dielectric constant decreased; the conductive polymer thus provided the softening effect under electric field. In the deflection response, the dielectrophoresis force and deflection distance increased monotonically with electric field strength, where the pure SF hydrogel showed the highest deflection distance and dielectrophoresis force. Copyright © 2015 Elsevier B.V. All rights reserved.

Dynamic Manipulation of Hydrogels to Control Cell Behavior: A Review

PubMed Central

Vats, Kanika

2013-01-01

For many tissue engineering applications and studies to understand how materials fundamentally affect cellular functions, it is important to have the ability to synthesize biomaterials that can mimic elements of native cell–extracellular matrix interactions. Hydrogels possess many properties that are desirable for studying cell behavior. For example, hydrogels are biocompatible and can be biochemically and mechanically altered by exploiting the presentation of cell adhesive epitopes or by changing hydrogel crosslinking density. To establish physical and biochemical tunability, hydrogels can be engineered to alter their properties upon interaction with external driving forces such as pH, temperature, electric current, as well as exposure to cytocompatible irradiation. Additionally, hydrogels can be engineered to respond to enzymes secreted by cells, such as matrix metalloproteinases and hyaluronidases. This review details different strategies and mechanisms by which biomaterials, specifically hydrogels, can be manipulated dynamically to affect cell behavior. By employing the appropriate combination of stimuli and hydrogel composition and architecture, cell behavior such as adhesion, migration, proliferation, and differentiation can be controlled in real time. This three-dimensional control in cell behavior can help create programmable cell niches that can be useful for fundamental cell studies and in a variety of tissue engineering applications. PMID:23541134

Preparation and properties of graphene oxide-regenerated cellulose/polyvinyl alcohol hydrogel with pH-sensitive behavior.

PubMed

Rui-Hong, Xie; Peng-Gang, Ren; Jian, Hui; Fang, Ren; Lian-Zhen, Ren; Zhen-Feng, Sun

2016-03-15

In this study, graphene oxide reinforced regenerated cellulose/polyvinyl alcohol (GO-RCE/PVA) ternary hydrogels were successfully prepared via a repeated freezing and thawing method in NaOH/urea aqueous solution. The effect of GO content on the mechanical properties, swelling behavior, water content of composite hydrogels was investigated. It was found that the mechanical properties of GO-RCE/PVA ternary hydrogels were largely enhanced relative to RCE/PVA hydrogels. With the addition of 1.0wt% GO, the tensile strength was increased by 40.4% from 0.52MPa to 0.73MPa, accompanied by the increase of the elongation at break (from 103% to 238%). Meanwhile, GO-RCE/PVA ternary hydrogels performed the excellent pH-sensitivity, and the higher pH leaded to higher swelling ratio. With 0.8wt% GO loading, the swelling ratio of GO-RCE/PVA ternary hydrogel was improved from 150% (pH=2) to 310% (pH=14). In addition, a slight increase in the water content of the ternary hydrogel was achieved with increasing concentrations of GO. It is believed that this novel ternary hydrogels is a promising material in the application of biomedical engineering and intelligent devices. Copyright © 2015 Elsevier Ltd. All rights reserved.

Polymeric hydrogels for novel contact lens-based ophthalmic drug delivery systems: a review.

PubMed

Xinming, Li; Yingde, Cui; Lloyd, Andrew W; Mikhalovsky, Sergey V; Sandeman, Susan R; Howel, Carol A; Liewen, Liao

2008-04-01

Only about 5% of drugs administrated by eye drops are bioavailable, and currently eye drops account for more than 90% of all ophthalmic formulations. The bioavailability of ophthalmic drugs can be improved by a soft contact lens-based ophthalmic drug delivery system. Several polymeric hydrogels have been investigated for soft contact lens-based ophthalmic drug delivery systems: (i) polymeric hydrogels for conventional contact lens to absorb and release ophthalmic drugs; (ii) polymeric hydrogels for piggyback contact lens combining with a drug plate or drug solution; (iii) surface-modified polymeric hydrogels to immobilize drugs on the surface of contact lenses; (iv) polymeric hydrogels for inclusion of drugs in a colloidal structure dispersed in the lens; (v) ion ligand-containing polymeric hydrogels; (vi) molecularly imprinted polymeric hydrogels which provide the contact lens with a high affinity and selectivity for a given drug. Polymeric hydrogels for these contact lens-based ophthalmic drug delivery systems, their advantages and drawbacks are critically analyzed in this review.

Effect of glycerol on sustained insulin release from PVA hydrogels and its application in diabetes therapy

PubMed Central

Cai, Yunpeng; Che, Junyi; Yuan, Minglu; Shi, Xiaohong; Chen, Wei; Yuan, Wei-En

2016-01-01

The present study aimed to investigate the effects of glycerol on the physical properties and release of an insulin-loaded polyvinyl alcohol (PVA) hydrogel film. The insulin-loaded hydrogel composite film was produced using the freeze-thawing method, after which the in vitro swelling ratio, transmittance and insulin release, and the in vivo pharmacodynamics, of hydrogels containing various volumes of glycerol were investigated. The results demonstrated that the addition of glycerol reduced the swelling ratio and increased the softness of the PVA hydrogel film. An analysis of insulin release in vitro and of the hypoglycemic effects in rats demonstrated that the PVA hydrogel film had a sustained release of insulin and long-acting effect over 10 days. The results of the present study suggested that, as a hydrophilic plasticizer, glycerol was able to enhance the release of insulin in the early stage of release profile by enhancing the formation of water channels, although the total swelling ratio was decreased. Therefore, the insulin-loaded glycerol/PVA hydrogel film may be a promising sustained-release preparation for the treatment of diabetes. PMID:27698690

Platelet-rich plasma loaded in situ-formed hydrogel enhances hyaline cartilage regeneration by CB1 upregulation.

PubMed

Lee, Hye-Rim; Park, Kyung Min; Joung, Yoon Ki; Park, Ki Dong; Do, Sun Hee

2012-11-01

The efficacy of three-dimensional (3D) culture on the proliferation and maturation of chondrocytes seeded into a hydrogel scaffold was assessed. Three types of hydrogel were prepared for the 3D culture of primary isolated chondrocytes. Chondrocyte proliferation was assessed using a live/dead viability/cytotoxicity assay and semiquantitative RT-PCR after 3D culture in hydrogel. Cylindrical defects in the center of rat xyphoids were used for the implantation of platelet-rich plasma (PRP)/hydrogel composites. Rats were killed at day 7 postoperatively and evaluated histochemically and immunohistologically. Xyphoid chondrocytes proliferated well with time in hydrogels. In the PRP-containing hydrogels, xyphoid defects displayed early formation of chondroid matrix with massive peripheral infiltration of spindle cells. These results were consistent with Safranin-O staining for proteoglycans and immunohistochemistry for type II collagen. Gene expression analyses in vitro revealed aggrecan, type II collagen, and ChM-1 and CB1 upregulation by PRP/hydrogel. PRP/hydrogel provided a suitable environment for hyaline cartilaginous regeneration, leading to anti-inflammation by significant increase of CB1 and inhibiting vascular ingrowth via considerable upregulation of ChM-1. The results provide a valuable reference for the clinical application of hydrogel scaffolds for hyaline cartilage regeneration, as well as the use of autologous PRP to improve cellular proliferation and maturation of xyphoid repair. Copyright © 2012 Wiley Periodicals, Inc.

Design of Decorated Self-Assembling Peptide Hydrogels as Architecture for Mesenchymal Stem Cells

PubMed Central

Zamuner, Annj; Cavo, Marta; Scaglione, Silvia; Messina, Grazia Maria Lucia; Russo, Teresa; Gloria, Antonio; Marletta, Giovanni; Dettin, Monica

2016-01-01

Hydrogels from self-assembling ionic complementary peptides have been receiving a lot of interest from the scientific community as mimetic of the extracellular matrix that can offer three-dimensional supports for cell growth or can become vehicles for the delivery of stem cells, drugs or bioactive proteins. In order to develop a 3D “architecture” for mesenchymal stem cells, we propose the introduction in the hydrogel of conjugates obtained by chemoselective ligation between a ionic-complementary self-assembling peptide (called EAK) and three different bioactive molecules: an adhesive sequence with 4 Glycine-Arginine-Glycine-Aspartic Acid-Serine-Proline (GRGDSP) motifs per chain, an adhesive peptide mapped on h-Vitronectin and the growth factor Insulin-like Growth Factor-1 (IGF-1). The mesenchymal stem cell adhesion assays showed a significant increase in adhesion and proliferation for the hydrogels decorated with each of the synthesized conjugates; moreover, such functionalized 3D hydrogels support cell spreading and elongation, validating the use of this class of self-assembly peptides-based material as very promising 3D model scaffolds for cell cultures, at variance of the less realistic 2D ones. Furthermore, small amplitude oscillatory shear tests showed that the presence of IGF-1-conjugate did not alter significantly the viscoelastic properties of the hydrogels even though differences were observed in the nanoscale structure of the scaffolds obtained by changing their composition, ranging from long, well-defined fibers for conjugates with adhesion sequences to the compact and dense film for the IGF-1-conjugate. PMID:28773852

Development of a thermosensitive HAMA-containing bio-ink for the fabrication of composite cartilage repair constructs.

PubMed

Mouser, V H M; Abbadessa, A; Levato, R; Hennink, W E; Vermonden, T; Gawlitta, D; Malda, J

2017-03-23

Fine-tuning of bio-ink composition and material processing parameters is crucial for the development of biomechanically relevant cartilage constructs. This study aims to design and develop cartilage constructs with tunable internal architectures and relevant mechanical properties. More specifically, the potential of methacrylated hyaluronic acid (HAMA) added to thermosensitive hydrogels composed of methacrylated poly[N-(2-hydroxypropyl)methacrylamide mono/dilactate] (pHPMA-lac)/polyethylene glycol (PEG) triblock copolymers, to optimize cartilage-like tissue formation by embedded chondrocytes, and enhance printability was explored. Additionally, co-printing with polycaprolactone (PCL) was performed for mechanical reinforcement. Chondrocyte-laden hydrogels composed of pHPMA-lac-PEG and different concentrations of HAMA (0%-1% w/w) were cultured for 28 d in vitro and subsequently evaluated for the presence of cartilage-like matrix. Young's moduli were determined for hydrogels with the different HAMA concentrations. Additionally, hydrogel/PCL constructs with different internal architectures were co-printed and analyzed for their mechanical properties. The results of this study demonstrated a dose-dependent effect of HAMA concentration on cartilage matrix synthesis by chondrocytes. Glycosaminoglycan (GAG) and collagen type II content increased with intermediate HAMA concentrations (0.25%-0.5%) compared to HAMA-free controls, while a relatively high HAMA concentration (1%) resulted in increased fibrocartilage formation. Young's moduli of generated hydrogel constructs ranged from 14 to 31 kPa and increased with increasing HAMA concentration. The pHPMA-lac-PEG hydrogels with 0.5% HAMA were found to be optimal for cartilage-like tissue formation. Therefore, this hydrogel system was co-printed with PCL to generate porous or solid constructs with different mesh sizes. Young's moduli of these composite constructs were in the range of native cartilage (3.5-4.6 MPa). Interestingly, the co-printing procedure influenced the mechanical properties of the final constructs. These findings are relevant for future bio-ink development, as they demonstrate the importance of selecting proper HAMA concentrations, as well as appropriate print settings and construct designs for optimal cartilage matrix deposition and final mechanical properties of constructs, respectively.

Methacrylated gelatin/hyaluronan-based hydrogels for soft tissue engineering

PubMed Central

Kessler, Lukas; Gehrke, Sandra; Winnefeld, Marc; Huber, Birgit; Hoch, Eva; Walter, Torsten; Wyrwa, Ralf; Schnabelrauch, Matthias; Schmidt, Malte; Kückelhaus, Maximilian; Lehnhardt, Marcus; Hirsch, Tobias; Jacobsen, Frank

2017-01-01

In vitro–generated soft tissue could provide alternate therapies for soft tissue defects. The aim of this study was to evaluate methacrylated gelatin/hyaluronan as scaffolds for soft tissue engineering and their interaction with human adipose–derived stem cells (hASCs). ASCs were incorporated into methacrylated gelatin/hyaluronan hydrogels. The gels were photocrosslinked with a lithium phenyl-2,4,6-trimethylbenzoylphosphinate photoinitiator and analyzed for cell viability and adipogenic differentiation of ASCs over a period of 30 days. Additionally, an angiogenesis assay was performed to assess their angiogenic potential. After 24 h, ASCs showed increased viability on composite hydrogels. These results were consistent over 21 days of culture. By induction of adipogenic differentiation, the mature adipocytes were observed after 7 days of culture, their number significantly increased until day 28 as well as expression of fatty acid binding protein 4 and adiponectin. Our scaffolds are promising as building blocks for adipose tissue engineering and allowed long viability, proliferation, and differentiation of ASCs. PMID:29318000

Effect of freeze-thawing conditions for preparation of chitosan-poly (vinyl alcohol) hydrogels and drug release studies.

PubMed

Figueroa-Pizano, M D; Vélaz, I; Peñas, F J; Zavala-Rivera, P; Rosas-Durazo, A J; Maldonado-Arce, A D; Martínez-Barbosa, M E

2018-09-01

The freezing-thawing is an advantageous method to produce hydrogels without crosslinking agents. In this study chitosan-poly(vinyl alcohol) (CS-PVA) hydrogels were prepared by varying the freezing conditions and composition, which affect the final characteristics of the products. The swelling degree, morphology, porosity, and diflunisal drug loading, as well as the drug release profiles were evaluated. The hydrogel swelling ratio was found to be mainly affected by the CS content, the number of freezing cycles and the temperature. SEM micrographs and porosity data confirm that pore size increases with the chitosan content. However, the use of either lower temperatures or longer freezing times, results in higher porosity and smaller pores. The drug release times of the CS-PVA hydrogels were as long as 30 h, and according to the mathematical fitting, a simple diffusion mechanism dominates the process. Moreover, a mathematical model predicting the hydrogels physical and structural behavior is proposed. Copyright © 2018 Elsevier Ltd. All rights reserved.

Microscale Bioadhesive Hydrogel Arrays for Cell Engineering Applications.

PubMed

Patel, Ravi Ghanshyam; Purwada, Alberto; Cerchietti, Leandro; Inghirami, Giorgio; Melnick, Ari; Gaharwar, Akhilesh K; Singh, Ankur

2014-09-01

Bioengineered hydrogels have been explored in cell and tissue engineering applications to support cell growth and modulate its behavior. A rationally designed scaffold should allow for encapsulated cells to survive, adhere, proliferate, remodel the niche, and can be used for controlled delivery of biomolecules. Here we report a microarray of composite bioadhesive microgels with modular dimensions, tunable mechanical properties and bulk modified adhesive biomolecule composition. Composite bioadhesive microgels of maleimide functionalized polyethylene glycol (PEG-MAL) with interpenetrating network (IPN) of gelatin ionically cross-linked with silicate nanoparticles were engineered by integrating microfabrication with Michael-type addition chemistry and ionic gelation. By encapsulating clinically relevant anchorage-dependent cervical cancer cells and suspension leukemia cells as cell culture models in these composite microgels, we demonstrate enhanced cell spreading, survival, and metabolic activity compared to control gels. The composite bioadhesive hydrogels represent a platform that could be used to study independent effect of stiffness and adhesive ligand density on cell survival and function. We envision that such microarrays of cell adhesive microenvironments, which do not require harsh chemical and UV crosslinking conditions, will provide a more efficacious cell culture platform that can be used to study cell behavior and survival, function as building blocks to fabricate 3D tissue structures, cell delivery systems, and high throughput drug screening devices.

Microscale Bioadhesive Hydrogel Arrays for Cell Engineering Applications

PubMed Central

PATEL, RAVI GHANSHYAM; PURWADA, ALBERTO; CERCHIETTI, LEANDRO; INGHIRAMI, GIORGIO; MELNICK, ARI; GAHARWAR, AKHILESH K.; SINGH, ANKUR

2014-01-01

Bioengineered hydrogels have been explored in cell and tissue engineering applications to support cell growth and modulate its behavior. A rationally designed scaffold should allow for encapsulated cells to survive, adhere, proliferate, remodel the niche, and can be used for controlled delivery of biomolecules. Here we report a microarray of composite bioadhesive microgels with modular dimensions, tunable mechanical properties and bulk modified adhesive biomolecule composition. Composite bioadhesive microgels of maleimide functionalized polyethylene glycol (PEG-MAL) with interpenetrating network (IPN) of gelatin ionically cross-linked with silicate nanoparticles were engineered by integrating microfabrication with Michael-type addition chemistry and ionic gelation. By encapsulating clinically relevant anchorage-dependent cervical cancer cells and suspension leukemia cells as cell culture models in these composite microgels, we demonstrate enhanced cell spreading, survival, and metabolic activity compared to control gels. The composite bioadhesive hydrogels represent a platform that could be used to study independent effect of stiffness and adhesive ligand density on cell survival and function. We envision that such microarrays of cell adhesive microenvironments, which do not require harsh chemical and UV crosslinking conditions, will provide a more efficacious cell culture platform that can be used to study cell behavior and survival, function as building blocks to fabricate 3D tissue structures, cell delivery systems, and high throughput drug screening devices. PMID:25328548

Timolol maleate release from hyaluronic acid-containing model silicone hydrogel contact lens materials.

PubMed

Korogiannaki, Myrto; Guidi, Giuliano; Jones, Lyndon; Sheardown, Heather

2015-09-01

This study was designed to assess the impact of a releasable wetting agent, such as hyaluronic acid (HA), on the release profile of timolol maleate (TM) from model silicone hydrogel contact lens materials. Polyvinylpyrrolidone (PVP) was used as an alternative wetting agent for comparison. The model lenses consisted of a hydrophilic monomer, either 2-hydroxyethyl methacrylate or N,N-dimethylacrylamide and a hydrophobic silicone monomer of methacryloxypropyltris (trimethylsiloxy) silane. The loading of the wetting and the therapeutic agent occurred during the synthesis of the silicone hydrogels through the method of direct entrapment. The developed materials were characterized by minimal changes in the water uptake, while lower molecular weight of HA improved their surface wettability. The transparency of the examined silicone hydrogels was found to be affected by the miscibility of the wetting agent in the prepolymer mixture as well as the composition of the developed silicone hydrogels. Sustained release of TM from 4 to 14 days was observed, with the drug transport occurring presumably through the hydrophilic domains of the silicone hydrogels. The release profile was strongly dependent on the hydrophilic monomer composition, the distribution of hydrophobic (silane) domains, and the affinity of the therapeutic agent for the silicone hydrogel matrix. Noncovalent entrapment of the wetting agent did not change the in vitro release duration and kinetics of TM, however the drug release profile was found to be controlled by the simultaneous release of TM and HA or PVP. In the case of HA, depending on the HA:drug ratio, the release rate was decreased and controlled by the release of HA, likely due to electrostatic interactions between protonated TM and anionic HA. Overall, partitioning of the drug within the hydrophilic domains of the silicone hydrogels as well as interactions with the wetting agent determined the drug release profile. © The Author(s) 2015.

A PEGylated platelet free plasma hydrogel based composite scaffold enables stable vascularization and targeted cell delivery for volumetric muscle loss.

PubMed

Aurora, Amit; Wrice, Nicole; Walters, Thomas J; Christy, Robert J; Natesan, Shanmugasundaram

2018-01-01

Extracellular matrix (ECM) scaffolds are being used for the clinical repair of soft tissue injuries. Although improved functional outcomes have been reported, ECM scaffolds show limited tissue specific remodeling response with concomitant deposition of fibrotic tissue. One plausible explanation is the regression of blood vessels which may be limiting the diffusion of oxygen and nutrients across the scaffold. Herein we develop a composite scaffold as a vasculo-inductive platform by integrating PEGylated platelet free plasma (PFP) hydrogel with a muscle derived ECM scaffold (m-ECM). In vitro, adipose derived stem cells (ASCs) seeded onto the composite scaffold differentiated into two distinct morphologies, a tubular network in the hydrogel, and elongated structures along the m-ECM scaffold. The composite scaffold showed a high expression of ITGA5, ITGB1, and FN and a synergistic up-regulation of ang1 and tie-2 transcripts. The in vitro ability of the composite scaffold to provide extracellular milieu for cell adhesion and molecular cues to support vessel formation was investigated in a rodent volumetric muscle loss (VML) model. The composite scaffold delivered with ASCs supported robust and stable vascularization. Additionally, the composite scaffold supported increased localization of ASCs in the defect demonstrating its ability for localized cell delivery. Interestingly, ASCs were observed homing in the injured muscle and around the perivascular space possibly to stabilize the host vasculature. In conclusion, the composite scaffold delivered with ASCs presents a promising approach for scaffold vascularization. The versatile nature of the composite scaffold also makes it easily adaptable for the repair of soft tissue injuries. Decellularized extracellular matrix (ECM) scaffolds when used for soft tissue repair is often accompanied by deposition of fibrotic tissue possibly due to limited scaffold vascularization, which limits the diffusion of oxygen and nutrients across the scaffold. Although a variety of scaffold vascularization strategies has been investigated, their limitations preclude rapid clinical translation. In this study we have developed a composite scaffold by integrating bi-functional polyethylene glycol modified platelet free plasma (PEGylated PFP) with adipose derived stem cells (ASCs) along with a muscle derived ECM scaffold (m-ECM). The composite scaffold provides a vasculo-inductive and an effective cell delivery platform for volumetric muscle loss. Copyright © 2017 Acta Materialia Inc. All rights reserved.

Cellulose-pectin composite hydrogels: Intermolecular interactions and material properties depend on order of assembly.

PubMed

Lopez-Sanchez, Patricia; Martinez-Sanz, Marta; Bonilla, Mauricio R; Wang, Dongjie; Gilbert, Elliot P; Stokes, Jason R; Gidley, Michael J

2017-04-15

Plant cell walls have a unique combination of strength and flexibility however, further investigations are required to understand how those properties arise from the assembly of the relevant biopolymers. Recent studies indicate that Ca 2+ -pectates can act as load-bearing components in cell walls. To investigate this proposed role of pectins, bioinspired wall models were synthesised based on bacterial cellulose containing pectin-calcium gels by varying the order of assembly of cellulose/pectin networks, pectin degree of methylesterification and calcium concentration. Hydrogels in which pectin-calcium assembly occurred prior to cellulose synthesis showed evidence for direct cellulose/pectin interactions from small-angle scattering (SAXS and SANS), had the densest networks and the lowest normal stress. The strength of the pectin-calcium gel affected cellulose structure, crystallinity and material properties. The results highlight the importance of the order of assembly on the properties of cellulose composite networks and support the role of pectin in the mechanics of cell walls. Copyright © 2017 Elsevier Ltd. All rights reserved.

Biomimetic hydrogels gate transport of calcium ions across cell culture inserts.

PubMed

Kotanen, Christian N; Wilson, A Nolan; Wilson, Ann M; Ishihara, Kazuhiko; Guiseppi-Elie, Anthony

2012-06-01

Control of the in vitro spatiotemporal availability of calcium ions is one means by which the microenvironments of hematopoietic stem cells grown in culture may be reproduced. The effects of cross-linking density on the diffusivity of calcium ions through cell culture compatible poly(2-hydroxyethyl methacrylate) [poly(HEMA)]-based bioactive hydrogels possessing 1.0 mol% 2-methacryloyloxyethyl phosphorylcholine (MPC), 5 mol% N,N-(dimethylamino)ethylmethacrylate (DMAEMA) and ca. 17 mol% n-butyl acrylate (n-BA) have been investigated to determine if varying cross-link density is a viable approach to controlling transport of calcium across hydrogel membranes. Cross-linking density was varied by changing the composition of cross-linker, tetraethyleneglycol diacrylate (TEGDA). The hydrogel membranes were formed by sandwich casting onto the external surface of track-etched polycarbonate membranes (T = 10 μm, φ = 0.4 μm pores) of cell culture inserts, polymerized in place by UV light irradiation and immersed in buffered (0.025 HEPES, pH 7.4) 0.10 M calcium chloride solution. The transport of calcium ions across the hydrogel membrane was monitored using a calcium ion selective electrode set within the insert. Degree of hydration (21.6 ± 1.0%) and void fraction were found to be constant across all cross-linking densities. Diffusion coefficients, determined using time-lag analysis, were shown to be strongly dependent on and to exponentially decrease with increasing cross-linking density. Compared to that found in buffer (2.0-2.5 × 10⁻⁶ cm²/s), diffusion coefficients ranged from 1.40 × 10⁻⁶ cm²/s to 1.80 × 10⁻⁷ cm²/s and tortuosity values ranged from 1.7 to 10.0 for the 1 and 12 mol% TEGDA cross-linked hydrogels respectively. Changes in tortuosity arising from variations in cross-link density were found to be the primary modality for controlling diffusivity through novel n-BA containing poly(HEMA)-based bioactive hydrogels.

Photo-crosslinked PDMSstar-PEG Hydrogels: Synthesis, Characterization, and Potential Application for Tissue Engineering Scaffolds

PubMed Central

Hou, Yaping; Schoener, Cody A.; Regan, Katherine R.; Munoz-Pinto, Dany; Hahn, Mariah S.; Grunlan, Melissa A.

2010-01-01

Inorganic-organic hydrogels with tunable chemical and physical properties were prepared from methacrylated star polydimethylsiloxane (PDMSstar-MA) and diacrylated poly(ethylene glycol) (PEG-DA) for use as tissue engineering scaffolds. Eighteen compositionally unique hydrogels were prepared by photo-crosslinking varying weight ratios of PEG-DA and PDMSstar-MA of different molecular weights (Mn): PEG-DA (Mn = 3.4k and 6k g/mol) and PDMSstar-MA (Mn = 1.8k, 5k and 7k g/mol). Introduction of PDMSstar-MA caused formation of discrete PDMS-enriched microparticles dispersed within the PEG matrix. The swelling ratio, mechanical properties in tension and compression, non-specific protein adhesion, controlled introduction of bioactivity and cytotoxicity of hydrogels were studied. This library of inorganic-organic hydrogels with tunable properties provides a useful platform to study the effect of scaffold properties on cell behavior. PMID:20146518

Fabrication of Self-Healable and Patternable Polypyrrole/Agarose Hybrid Hydrogels for Smart Bioelectrodes.

PubMed

Park, Nokyoung; Chae, Seung Chul; Kim, Il Tae; Hur, Jaehyun

2016-02-01

We present a new class of electrically conductive, mechanically moldable, and thermally self-healable hybrid hydrogels. The hybrid gels consist of polypyrrole and agarose as the conductive component and self-healable matrix, respectively. By using the appropriate oxidizing agent under conditions of mild temperature, the polymerization of pyrrole occurred along the three-dimensional network of the agarose hydrogel matrix. In contrast to most commercially available hydrogels, the physical crosslinking of agarose gel allows for reversible gelation in the case of our hybrid gel, which could be manipulated by temperature variation, which controls the electrical on/off behavior of the hybrid gel electrode. Exploiting this property, we fabricated a hybrid conductive hydrogel electrode which also self-heals thermally. The novel composite material we report here will be useful for many technological and biological applications, especially in reactive biomimetic functions and devices, artificial muscles, smart membranes, smart full organic batteries, and artificial chemical synapses.

Spider Silks-Biomimetics Beyond Silk Fibers: Hydrogels, films & Adhesives from Aqueous Recombinant Spider Silk dopes: A Synchrotron X-Ray Nano-Structural Study

NASA Astrophysics Data System (ADS)

Sampath, Sujatha; Jones, Justin; Harris, Thomas; Lewis, Randolph

2015-03-01

With a combination of high strength and extensibility, spider silk's (SS) mechanical properties surpass those of any man made fiber. The superior properties are due to the primary protein composition and the complex hierarchical structural organization from nanoscale to macroscopic length scales. Considerable progress has been made to synthetically mimic the production of fibers based on SS proteins. We present synchrotron x-ray micro diffraction (SyXRD) results on new fibers and gels (hydrogels, lyogels) from recombinant SS protein water-soluble dopes. Novelty in these materials is two-fold: water based rather than widely used HFIP acid synthesis, makes them safe in medical applications (replacement for tendons & ligaments). Secondly, hydrogels morphology render them as excellent carriers for targeted drug delivery biomedical applications. SyXRD results reveal semi-crystalline structure with ordered beta-sheets and relatively high degree of axial orientation in the fibers, making them the closest yet to natural spider silks. SyXRD on the gels elucidate the structural transformations during the self-recovery process through mechanical removal and addition of water. Studies correlating the observed structural changes to mechanical properties are underway.

Development of soy lecithin based novel self-assembled emulsion hydrogels.

PubMed

Singh, Vinay K; Pandey, Preeti M; Agarwal, Tarun; Kumar, Dilip; Banerjee, Indranil; Anis, Arfat; Pal, Kunal

2015-03-01

The current study reports the development and characterization of soy lecithin based novel self-assembled emulsion hydrogels. Sesame oil was used as the representative oil phase. Emulsion gels were formed when the concentration of soy lecithin was >40% w/w. Metronidazole was used as the model drug for the drug release and the antimicrobial tests. Microscopic study showed the apolar dispersed phase in an aqueous continuum phase, suggesting the formation of emulsion hydrogels. FTIR study indicated the formation of intermolecular hydrogen bonding, whereas, the XRD study indicated predominantly amorphous nature of the emulsion gels. Composition dependent mechanical and drug release properties of the emulsion gels were observed. In-depth analyses of the mechanical studies were done using Ostwald-de Waele power-law, Kohlrausch and Weichert models, whereas, the drug release profiles were modeled using Korsmeyer-Peppas and Peppas-Sahlin models. The mechanical analyses indicated viscoelastic nature of the emulsion gels. The release of the drug from the emulsion gels was diffusion mediated. The drug loaded emulsion gels showed good antimicrobial activity. The biocompatibility test using HaCaT cells (human keratinocytes) suggested biocompatibility of the emulsion gels. Copyright © 2015 Elsevier Ltd. All rights reserved.

Silver nanoparticle based antibacterial methacrylate hydrogels potential for bone graft applications.

PubMed

González-Sánchez, M Isabel; Perni, Stefano; Tommasi, Giacomo; Morris, Nathanael Glyn; Hawkins, Karl; López-Cabarcos, Enrique; Prokopovich, Polina

2015-05-01

Infections are frequent and very undesired occurrences after orthopedic procedures; furthermore, the growing concern caused by the rise in antibiotic resistance is progressively dwindling the efficacy of such drugs. Artificial bone graft materials could solve some of the problems associated with the gold standard use of natural bone graft such as limited bone material, pain at the donor site and rejections if donor tissue is used. We have previously described new acrylate base nanocomposite hydrogels as bone graft materials. In the present paper, we describe the integration of silver nanoparticles in the polymeric mineralized biomaterial to provide non-antibiotic antibacterial activity against Staphylococcus epidermidis and Methicillin-resistant Staphylococcus aureus. Two different crosslinking degrees were tested and the silver nanoparticles were integrated into the composite matrix by means of three different methods: entrapment in the polymeric hydrogel before the mineralization; diffusion during the process of calcium phosphate crystallization and adsorption post-mineralization. The latter being generally the most effective method of encapsulation; however, the adsorption of silver nanoparticles inside the pores of the biomaterial led to a decreasing antibacterial activity for adsorption time longer than 2 days. Copyright © 2015. Published by Elsevier B.V.

Bio-based topical system for enhanced salicylic acid delivery: preparation and performance of gels.

PubMed

Langasco, Rita; Spada, Gianpiera; Tanriverdi, Sakine Tuncay; Rassu, Giovanna; Giunchedi, Paolo; Özer, Özgen; Gavini, Elisabetta

2016-08-01

New salicylic acid (SA)-loaded gels were developed using excipients made from renewable materials, and our goal was to improve drug permeation in the topical treatment of acne vulgaris. We studied the preparation parameters to obtain suitable gel formulations. Only naturally occurring polymers were used as gelling agents. Two hydrogels and three lipogels were selected and characterized in terms of drug loading, pH, viability cells, rheology, mechanical properties and in vitro permeation; these hydrogels and lipogels were compared with the traditional ointment. We also evaluated skin parameters before and after gel application. The formulations that we studied are non-Newtonian fluids; they have high drug loading and suitable mechanical properties. Lipogels exhibit a slower and more linear in vitro permeation profile compared with hydrogels. The different vehicles that we used affected drug permeation and improve patient compliance. Cytotoxicity studies suggest that all of the formulations are non-toxic. Lipogels demonstrate appropriate technological features and improved performance compared with the traditional ointment with regard to their composition. Lipogels may represent a new bio-based topical system for SA delivery. The use of 'green' excipients leads to 'skin-friendly' formulations that are able to satisfy environmental safety. © 2016 Royal Pharmaceutical Society.

Silver nanoparticle based antibacterial methacrylate hydrogels potential for bone graft applications

PubMed Central

González-Sánchez, M. Isabel; Perni, Stefano; Tommasi, Giacomo; Morris, Nathanael Glyn; Hawkins, Karl; López-Cabarcos, Enrique; Prokopovich, Polina

2015-01-01

Infections are frequent and very undesired occurrences after orthopedic procedures; furthermore, the growing concern caused by the rise in antibiotic resistance is progressively dwindling the efficacy of such drugs. Artificial bone graft materials could solve some of the problems associated with the gold standard use of natural bone graft such as limited bone material, pain at the donor site and rejections if donor tissue is used. We have previously described new acrylate base nanocomposite hydrogels as bone graft materials. In the present paper, we describe the integration of silver nanoparticles in the polymeric mineralized biomaterial to provide non-antibiotic antibacterial activity against Staphylococcus epidermidis and Methicillin-resistant Staphylococcus aureus. Two different crosslinking degrees were tested and the silver nanoparticles were integrated into the composite matrix by means of three different methods: entrapment in the polymeric hydrogel before the mineralization; diffusion during the process of calcium phosphate crystallization and adsorption post-mineralization. The latter being generally the most effective method of encapsulation; however, the adsorption of silver nanoparticles inside the pores of the biomaterial led to a decreasing antibacterial activity for adsorption time longer than 2 days. PMID:25746278

Nanosized ethosomes-based hydrogel formulations of methoxsalen for enhanced topical delivery against vitiligo: formulation optimization, in vitro evaluation and preclinical assessment.

PubMed

Garg, Bhawna Jain; Garg, Neeraj K; Beg, Sarwar; Singh, Bhupinder; Katare, Om Prakash

2016-01-01

The present investigation aimed for the development and characterization of ethosomes-based hydrogel formulations of methoxsalen for enhanced topical delivery and effective treatment against vitiligo. The ethosomes were prepared by central composite design (CCD) and characterized for various quality attributes like vesicle shape, size, zeta potential, lamellarity, drug entrapment and drug leaching. The optimized ethosomes were subsequently incorporated int Carbopol® 934 gel and characterized for drug content, rheological behavior, texture profile, in vitro release, ex vivo skin permeation and retention, skin photosensitization and histopathological examination. Ethosomes were found to be spherical and multilamellar in structures having nanometric size range with narrow size distribution, and high encapsulation efficiency. Ethosomal formulations showed significant skin permeation and accumulation in the epidermal and dermal layers. The fluorescence microscopy study using 123 Rhodamine exhibited enhanced permeation of the drug-loaded ethosomes in the deeper layers of skin. Also, the developed formulation showed insignificant phototoxicity and erythema vis-à-vis the conventional cream. The results were cross-validated using histopathological examination of skin segments. In a nutshell, the ethosomes-based hydrogel formulation was found to be a promising drug delivery system demonstrating enhanced percutaneous penetration of methoxsalen with reduced phototoxicity and erythema, thus leading to improved patient compliance for the treatment against vitiligo.

Xylan-Modified-Based Hydrogels with Temperature/pH Dual Sensitivity and Controllable Drug Delivery Behavior

PubMed Central

Kong, Wei-Qing; Gao, Cun-Dian; Hu, Shu-Feng; Ren, Jun-Li; Zhao, Li-Hong; Sun, Run-Cang

2017-01-01

Among the natural macromolecules potentially used as the scaffold material in hydrogels, xylan has aroused great interest in many fields because of its biocompatibility, low toxicity, and biodegradability. In this work, new pH and thermoresponsive hydrogels were prepared by the cross-linking polymerization of maleic anhydride-modified xylan (MAHX) with N-isopropylacrylamide (NIPAm) and acrylic acid (AA) under UV irradiation to form MAHX-g-P(NIPAm-co-AA) hydrogels. The pore volume, the mechanical properties, and the release rate for drugs of hydrogels could be controlled by the degree of substitution of MAHX. These hydrogels were characterized by swelling ability, lower critical solution temperature (LCST), Fourier-transform infrared (FTIR), and SEM. Furthermore, the cumulative release rate was investigated for acetylsalicylic acid and theophylline, as well as the cytocompatibility MAHX-based hydrogels. Results showed that MAHX-based hydrogels exhibited excellent swelling–deswelling properties, uniform porous structure, and the temperature/pH dual sensitivity. In vitro, the cumulative release rate of acetylsalicylic acid for MAHX-based hydrogels was higher than that for theophylline, and in the gastrointestinal sustained drug release study, the acetylsalicylic acid release rate was extremely slow during the initial 3 h in the gastric fluid (24.26%), and then the cumulative release rate reached to 90.5% after sustained release for 5 h in simulated intestinal fluid. The cytotoxicity experiment demonstrated that MAHX-based hydrogels could promote cell proliferation and had satisfactory biocompatibility with NIH3T3 cells. These results indicated that MAHX-based hydrogels, as new drug carriers, had favorable behavior for intestinal-targeted drug delivery. PMID:28772664

Hydrogels from feather keratin show higher viscoelastic properties and cell proliferation than those from hair and wool keratins.

PubMed

Esparza, Yussef; Bandara, Nandika; Ullah, Aman; Wu, Jianping

2018-09-01

Hydrogel prepared from keratin shows potential applications in tissue engineering. However, the importance of the keratin sources has not been considered. The objectives of this study were to characterize and compare the rheological (storage modulus), physical (porosity, pore size, swelling capacity, and water contact angle) and in vitro cell compatibility of hydrogel scaffolds prepared from various keratin sources. Keratins were characterized by means of their molecular weight, amino acid composition, thermal and conformational properties. Hydrogels from chicken feather keratins demonstrated substantially higher storage modulus (G') than hair and wool keratin hydrogels. However, higher swelling capacity (>3000%) was determined in hair and wool over feather keratin (1500%) hydrogels. Our results suggest that small molecular weight and β-sheet conformation of feather keratin (~10 kDa) facilitated the self-assembly of rigid hydrogels through disulfide bond re-oxidation. Whereas, high molecular weight (10-75 kDa) stretchable α-helix conformation in hair and wool keratins resulted in weaker hydrogels. The cell cultures using fibroblasts showed the highest proliferation rate on chicken feather keratin hydrogel scaffolds. After 15 days of culture, partial breakdown of keratin fibers was observed. Results indicate that stiffer avian keratins can be used to fabricate more mechanically robust biomaterials than mammalian keratins. Copyright © 2018 Elsevier B.V. All rights reserved.

The construction of 3D-engineered tissues composed of cells and extracellular matrices by hydrogel template approach.

PubMed

Matsusaki, Michiya; Yoshida, Hiroaki; Akashi, Mitsuru

2007-06-01

The three-dimensional (3D)-engineered tissues composed of only cells and extracellular matrices (ECM) were constructed by the hydrogel template approach. The disulfide-crosslinked poly(gamma-glutamic acid) hydrogels were prepared as a template hydrogel. These template hydrogels were easily decomposed under physiological conditions using reductants such as cysteine, glutathione and dithiothreitol by cleavage of disulfide crosslinkage to thiol groups. The decomposed polymers are soluble in cell culture medium. The cleaving of disulfide bond was determined by UV-vis and FT-IR spectroscopies. We successfully prepared the 3D-engineered tissues (thickness/diameter, 2mm/1cm) composed of mouse L929 fibroblast cells and ECM by the decomposition of only the template hydrogel with cysteine after 10 days 3D-cell culture on/in the template hydrogel. The size and thickness of the 3D-engineered tissues was completely transferred from the template hydrogel. The cultured L929 cells viability in the obtained engineered tissues was confirmed by a culture test, WST-1 method and LIVE/DEAD staining assay. The engineered tissue was self-standing and highly dense composite of the cultured cells and collagen produced by the cells. This hydrogel template approach may be useful as a new class of soft-tissue engineering technology to substitute a synthetic polymer scaffold to the ECM scaffold produced from the cultured cells.

3D bioprinting of scaffolds with living Schwann cells for potential nerve tissue engineering applications.

PubMed

Ning, Liqun; Sun, Haoying; Lelong, Tiphanie; Guilloteau, Romain; Zhu, Ning; Schreyer, David J; Chen, Daniel Xiongbiao

2018-06-18

Three-dimensional (3D) bioprinting of biomaterials shows great potential for producing cell-encapsulated scaffolds to repair nerves after injury or disease. For this, preparation of biomaterials and bioprinting itself are critical to create scaffolds with both biological and mechanical properties appropriate for nerve regeneration, yet remain unachievable. This paper presents our study on bioprinting Schwann cell-encapsulated scaffolds using composite hydrogels of alginate, fibrin, hyaluronic acid, and/or RGD peptide, for nerve tissue engineering applications. For the preparation of composite hydrogels, suitable hydrogel combinations were identified and prepared by adjusting the concentration of fibrin based on the morphological spreading of Schwann cells. In bioprinting, the effects of various printing process parameters (including the air pressure for dispensing, dispensing head movement speed, and crosslinking conditions) on printed structures were investigated and, by regulating these parameters, mechanically-stable scaffolds with fully interconnected pores were printed. The performance of Schwann cells within the printed scaffolds were examined in terms of viability, proliferation, orientation, and ability to produce laminin. Our results show that the printed scaffolds can promote the alignment of Schwann cells inside scaffolds and thus provide haptotactic cues to direct the extension of dorsal root ganglion neurites along the printed strands, demonstrating their great potential for applications in the field of nerve tissue engineering. © 2018 IOP Publishing Ltd.

Poly-l-Lactic Acid Nanofiber-Polyamidoamine Hydrogel Composites: Preparation, Properties, and Preliminary Evaluation as Scaffolds for Human Pluripotent Stem Cell Culturing.

PubMed

Gualandi, Chiara; Bloise, Nora; Mauro, Nicolò; Ferruti, Paolo; Manfredi, Amedea; Sampaolesi, Maurilio; Liguori, Anna; Laurita, Romolo; Gherardi, Matteo; Colombo, Vittorio; Visai, Livia; Focarete, Maria Letizia; Ranucci, Elisabetta

2016-10-01

Electrospun poly-l-lactic acid (PLLA) nanofiber mats carrying surface amine groups, previously introduced by nitrogen atmospheric pressure nonequilibrium plasma, are embedded into aqueous solutions of oligomeric acrylamide-end capped AGMA1, a biocompatible polyamidoamine with arg-gly-asp (RGD)-reminiscent repeating units. The resultant mixture is finally cured giving PLLA-AGMA1 hydrogel composites that absorb large amounts of water and, in the swollen state, are translucent, soft, and pliable, yet as strong as the parent PLLA mat. They do not split apart from each other when swollen in water and remain highly flexible and resistant, since the hydrogel portion is covalently grafted onto the PLLA nanofibers via the addition reaction of the surface amine groups to a part of the terminal acrylic double bonds of AGMA1 oligomers. Preliminary tested as scaffolds, the composites prove capable of maintaining short-term undifferentiated cultures of human pluripotent stem cells in feeder-free conditions. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A pH- and temperature-responsive bioresorbable injectable hydrogel based on polypeptide block copolymers for the sustained delivery of proteins in vivo.

PubMed

Turabee, Md Hasan; Thambi, Thavasyappan; Duong, Huu Thuy Trang; Jeong, Ji Hoon; Lee, Doo Sung

2018-02-27

Sustained delivery of protein therapeutics is limited owing to the fragile nature of proteins. Despite its great potential, delivery of proteins without any loss of bioactivity remains a challenge in the use of protein therapeutics in the clinic. To surmount this shortcoming, we report a pH- and temperature-responsive in situ-forming injectable hydrogel based on comb-type polypeptide block copolymers for the controlled delivery of proteins. Polypeptide block copolymers, composed of hydrophilic polyethylene glycol (PEG), temperature-responsive poly(γ-benzyl-l-glutamate) (PBLG), and pH-responsive oligo(sulfamethazine) (OSM), exhibit pH- and temperature-induced sol-to-gel transition behavior in aqueous solutions. Polypeptide block copolymers were synthesized by combining N-carboxyanhydride-based ring-opening polymerization and post-functionalization of the chain-end using N-hydroxy succinimide ester activated OSM. The physical properties of polypeptide-based hydrogels were tuned by varying the composition of temperature- and pH-responsive PBLG and OSM in block copolymers. Polypeptide block copolymers were non-toxic to human embryonic kidney cells at high concentrations (2000 μg mL -1 ). Subcutaneous administration of polypeptide block copolymer sols formed viscoelastic gel instantly at the back of Sprague-Dawley (SD) rats. The in vivo gels exhibited sustained degradation and were found to be bioresorbable in 6 weeks without any noticeable inflammation at the injection site. Anionic characteristics of hydrogels allow efficient loading of a cationic model protein, lysozyme, through electrostatic interaction. Lysozyme-loaded polypeptide block copolymer sols readily formed a viscoelastic gel in vivo and sustained lysozyme release for at least a week. Overall, the results demonstrate an elegant approach to control the release of certain charged proteins and open a myriad of therapeutic possibilities in protein therapeutics.

Formulation and optimization of virgin coconut oil with Tween-80 incorporated in gellan gum hydrogel

NASA Astrophysics Data System (ADS)

Muktar, Muhammad Zulhelmi; Rose, Laili bt Che; Amin, Khairul Anuar Mat

2017-09-01

The demand for wound care products especially advance and active wound care product are huge. Honey and virgin coconut oil (VCO) are well-known as an ancient treatment to treat wound with its great properties such as antibacterial, anti-inflammatory and anti-viral. In this study, the potential of VCO incorporated in gellan gum (GG) hydrogel was examined. A surfactant, Tween-80 was introduced to reduce the interfacial tension between VCO and water. Ternary phase diagram was constructed to get the microemulsion of VCO. The compositions of VCO and Tween-80 at stable region were chosen and incorporated in GG solution. The swelling, water vapor transmission rates (WVTR) and gel fraction were significantly affected by the composition of VCO. Higher amount of VCO in GG hydrogel increased the tensile strength and gel fraction at a cost of decreased in swelling and WVTR values.

Microparticles Produced by the Hydrogel Template Method for Sustained Drug Delivery

PubMed Central

Lu, Ying; Sturek, Michael; Park, Kinam

2014-01-01

Polymeric microparticles have been used widely for sustained drug delivery. Current methods of microparticle production can be improved by making homogeneous particles in size and shape, increasing the drug loading, and controlling the initial burst release. In the current study, the hydrogel template method was used to produce homogeneous poly(lactide-co-glycolide) (PLGA) microparticles and to examine formulation and process-related parameters. Poly(vinyl alcohol) (PVA) was used to make hydrogel templates. The parameters examined include PVA molecular weight, type of PLGA (as characterized by lactide content, inherent viscosity), polymer concentration, drug concentration and composition of solvent system. Three model compounds studied were risperidone, methylprednisolone acetate and paclitaxel. The ability of the hydrogel template method to produce microparticles with good conformity to template was dependent on molecular weight of PVA and viscosity of the PLGA solution. Drug loading and encapsulation efficiency were found to be influenced by PLGA lactide content, polymer concentration and composition of the solvent system. The drug loading and encapsulation efficiency were 28.7% and 82% for risperidone, 31.5% and 90% for methylprednisolone acetate, and 32.2 % and 92 % for paclitaxel, respectively. For all three drugs, release was sustained for weeks, and the in vitro release profile of risperidone was comparable to that of microparticles prepared using the conventional emulsion method. The hydrogel template method provides a new approach of manipulating microparticles. PMID:24333903

Addition of perfluorocarbons to alginate hydrogels significantly impacts molecular transport and fracture stress.

PubMed

White, Joseph C; Stoppel, Whitney L; Roberts, Susan C; Bhatia, Surita R

2013-02-01

Perfluorocarbons (PFCs) are used in biomaterial formulations to increase oxygen (O(2) ) tension and create a homogeneous O(2) environment in three-dimensional tissue constructs. It is unclear how PFCs affect mechanical and transport properties of the scaffold, which are critical for robustness, intracellular signaling, protein transport, and overall device efficacy. In this study, we investigate composite alginate hydrogels containing a perfluorooctyl bromide (PFOB) emulsion stabilized with Pluronic(®) F68 (F68). We demonstrate that PFC addition significantly affects biomaterial properties and performance. Solution and hydrogel mechanical properties and transport of representative hydrophilic (riboflavin), hydrophobic (methyl and ethyl paraben), and protein (bovine serum albumin, BSA) solutes were compared in alginate/F68 composite hydrogels with or without PFOB. Our results indicate that mechanical properties of the alginate/F68/PFOB hydrogels are not significantly affected under small strains, but a significant decrease fracture stress is observed. The effective diffusivity D(eff) of hydrophobic small molecules decreases with PFOB emulsion addition, yet the D(eff) of hydrophilic small molecules remained unaffected. For BSA, the D(eff) increased and the loading capacity decreased with PFOB emulsion addition. Thus, a trade-off between the desired increased O(2) supply provided by PFCs and the mechanical weakening and change in transport of cellular signals must be carefully considered in the design of biomaterials containing PFCs. Copyright © 2012 Wiley Periodicals, Inc.

The influence of natural deep eutectic solvents on bioactive natural products: studying interactions between a hydrogel model and Schisandra chinensis metabolites.

PubMed

Liu, Yang; Zhang, Yu; Chen, Shao-Nong; Friesen, J Brent; Nikolić, Dejan; Choules, Mary P; McAlpine, James B; Lankin, David C; Gemeinhart, Richard A; Pauli, Guido F

2018-06-01

Natural Deep Eutectic Solvent (NADES) species can exhibit unexpected solubilizing power for lipophilic molecules despite their simple composition: hydrophilic organic molecules and water. In the present study, the unique properties of NADES species were applied in combination with a model polymer system: a hydrophilic chitosan/alginate hydrogel. Briefly, NADES species (e.g., mannose-dimethylurea-water, 2:5:5, mole/mole) formed matrices to 1) dissolve lipophilic molecules (e.g., curcumin), 2) load lipophilic molecule(s) into the hydrogel, and 3) spontaneously vacate from the system. NADES species ubiquitously occur in natural sources, and a crude extract is a mixture of the NADES species and bioactive metabolites. Based on these ideas, we hypothesized that the crude extract may also allow the loading of natural bioactive molecules from a natural NADES species into (bio)hydrogel systems. To evaluate this hypothesis in vitro, Schisandra chinensis fruit extract was chosen as a representative mixture of lipophilic botanical molecules and hydrophilic NADES species. The results showed that the NADES matrix of S. chinensis was capable of loading at least three bioactive lignans (i.e., gomisin A, gomisin J, and angeloylgomisin H) into the polymer system. The lipophilic metabolites can subsequently be released from the hydrogel. The outcomes suggest that a unique drug delivery mechanism may exist in nature, thereby potentially improving the bioavailability of lipophilic metabolites through physicochemical interactions with the NADES. Copyright © 2018 Elsevier B.V. All rights reserved.

Polymers in the gut compress the colonic mucus hydrogel

PubMed Central

Datta, Sujit S.; Preska Steinberg, Asher

2016-01-01

Colonic mucus is a key biological hydrogel that protects the gut from infection and physical damage and mediates host–microbe interactions and drug delivery. However, little is known about how its structure is influenced by materials it comes into contact with regularly. For example, the gut abounds in polymers such as dietary fibers or administered therapeutics, yet whether such polymers interact with the mucus hydrogel, and if so, how, remains unclear. Although several biological processes have been identified as potential regulators of mucus structure, the polymeric composition of the gut environment has been ignored. Here, we demonstrate that gut polymers do in fact regulate mucus hydrogel structure, and that polymer–mucus interactions can be described using a thermodynamic model based on Flory–Huggins solution theory. We found that both dietary and therapeutic polymers dramatically compressed murine colonic mucus ex vivo and in vivo. This behavior depended strongly on both polymer concentration and molecular weight, in agreement with the predictions of our thermodynamic model. Moreover, exposure to polymer-rich luminal fluid from germ-free mice strongly compressed the mucus hydrogel, whereas exposure to luminal fluid from specific-pathogen-free mice—whose microbiota degrade gut polymers—did not; this suggests that gut microbes modulate mucus structure by degrading polymers. These findings highlight the role of mucus as a responsive biomaterial, and reveal a mechanism of mucus restructuring that must be integrated into the design and interpretation of studies involving therapeutic polymers, dietary fibers, and fiber-degrading gut microbes. PMID:27303035

Polymers in the gut compress the colonic mucus hydrogel.

PubMed

Datta, Sujit S; Preska Steinberg, Asher; Ismagilov, Rustem F

2016-06-28

Colonic mucus is a key biological hydrogel that protects the gut from infection and physical damage and mediates host-microbe interactions and drug delivery. However, little is known about how its structure is influenced by materials it comes into contact with regularly. For example, the gut abounds in polymers such as dietary fibers or administered therapeutics, yet whether such polymers interact with the mucus hydrogel, and if so, how, remains unclear. Although several biological processes have been identified as potential regulators of mucus structure, the polymeric composition of the gut environment has been ignored. Here, we demonstrate that gut polymers do in fact regulate mucus hydrogel structure, and that polymer-mucus interactions can be described using a thermodynamic model based on Flory-Huggins solution theory. We found that both dietary and therapeutic polymers dramatically compressed murine colonic mucus ex vivo and in vivo. This behavior depended strongly on both polymer concentration and molecular weight, in agreement with the predictions of our thermodynamic model. Moreover, exposure to polymer-rich luminal fluid from germ-free mice strongly compressed the mucus hydrogel, whereas exposure to luminal fluid from specific-pathogen-free mice-whose microbiota degrade gut polymers-did not; this suggests that gut microbes modulate mucus structure by degrading polymers. These findings highlight the role of mucus as a responsive biomaterial, and reveal a mechanism of mucus restructuring that must be integrated into the design and interpretation of studies involving therapeutic polymers, dietary fibers, and fiber-degrading gut microbes.

Lecithin-based nanostructured gels for skin delivery: an update on state of art and recent applications.

PubMed

Elnaggar, Yosra S R; El-Refaie, Wessam M; El-Massik, Magda A; Abdallah, Ossama Y

2014-04-28

Conventional carriers for skin delivery encounter obstacles of drug leakage, scanty permeation and low entrapment efficiency. Phospholipid nanogels have recently been recognized as prominent delivery systems to circumvent such obstacles and impart easier application. The current review provides an overview on different types of lecithin nanostructured gels, with particular emphasis on liposomal versus microemulsion gelled systems. Liposomal gels investigated encompassed classic liposomal hydrogel, modified liposomal gels (e.g. Transferosomal, Ethosomal, Pro-liposomal and Phytosomal gels), Microgel in liposomes (M-i-L) and Vesicular phospholipid gel (VPG). Microemulsion gelled systems encompassed Lecithin microemulsion-based organogels (LMBGs), Pluronic lecithin organogels (PLOs) and Lecithin-stabilized microemulsion-based hydrogels. All systems were reviewed regarding matrix composition, state of art, characterization and updated applications. Different classes of lecithin nanogels exhibited crucial impact on transdermal delivery regarding drug permeation, drug loading and stability aspects. Future perspectives of this theme issue are discussed based on current laboratory studies. Copyright © 2014 Elsevier B.V. All rights reserved.

Protease-modulating polyacrylate-based hydrogel stimulates wound bed preparation in venous leg ulcers – a randomized controlled trial

PubMed Central

Humbert, P; Faivre, B; Véran, Y; Debure, C; Truchetet, F; Bécherel, P-A; Plantin, P; Kerihuel, J-C; Eming, SA; Dissemond, J; Weyandt, G; Kaspar, D; Smola, H; Zöllner, P

2014-01-01

Background Stringent control of proteolytic activity represents a major therapeutic approach for wound-bed preparation. Objectives We tested whether a protease-modulating polyacrylate- (PA-) containing hydrogel resulted in a more efficient wound-bed preparation of venous leg ulcers when compared to an amorphous hydrogel without known protease-modulating properties. Methods Patients were randomized to the polyacrylate-based hydrogel (n = 34) or to an amorphous hydrogel (n = 41). Wound beds were evaluated by three blinded experts using photographs taken on days 0, 7 and 14. Results After 14 days of treatment there was an absolute decrease in fibrin and necrotic tissue of 37.6 ± 29.9 percentage points in the PA-based hydrogel group and by 16.8 ± 23.0 percentage points in the amorphous hydrogel group. The absolute increase in the proportion of ulcer area covered by granulation tissue was 36.0 ± 27.4 percentage points in the PA-based hydrogel group and 14.5 ± 22.0 percentage points in the control group. The differences between the groups were significant (decrease in fibrin and necrotic tissue P = 0.004 and increase in granulation tissue P = 0.0005, respectively). Conclusion In particular, long-standing wounds profited from the treatment with the PA-based hydrogel. These data suggest that PA-based hydrogel dressings can stimulate normalization of the wound environment, particularly in hard-to-heal ulcers. PMID:24612304

Super-tough, ultra-stretchable and strongly compressive hydrogels with core-shell latex particles inducing efficient aggregation of hydrophobic chains.

PubMed

Ren, Xiuyan; Huang, Chang; Duan, Lijie; Liu, Baijun; Bu, Lvjun; Guan, Shuang; Hou, Jiliang; Zhang, Huixuan; Gao, Guanghui

2017-05-14

Toughness, strechability and compressibility for hydrogels were ordinarily balanced for their use as mechanically responsive materials. For example, macromolecular microsphere composite hydrogels with chemical crosslinking exhibited excellent compression strength and strechability, but poor tensile stress. Here, a novel strategy for the preparation of a super-tough, ultra-stretchable and strongly compressive hydrogel was proposed by introducing core-shell latex particles (LPs) as crosslinking centers for inducing efficient aggregation of hydrophobic chains. The core-shell LPs always maintained a spherical shape due to the presence of a hard core even by an external force and the soft shell could interact with hydrophobic chains due to hydrophobic interactions. As a result, the hydrogels reinforced by core-shell LPs exhibited not only a high tensile strength of 1.8 MPa and dramatic elongation of over 20 times, but also an excellent compressive performance of 13.5 MPa at a strain of 90%. The Mullins effect was verified for the validity of core-shell LP-reinforced hydrogels by inducing aggregation of hydrophobic chains. The novel strategy strives to provide a better avenue for designing and developing a new generation of hydrophobic association tough hydrogels with excellent mechanical properties.

Graphene Based Nanomaterials: Synthesis and the Structural Applications

NASA Astrophysics Data System (ADS)

Cao, Linlin

Along with the development of nanomaterials and nanotechnology, graphene has attracted great attention due to its outstanding mechanical, electrical, and physical properties. Graphene oxide (GO), as a derivative of graphene, has also attracted great attention, especially as reinforcements for strong and lightweight composites. The most widely used method to synthesize GO is Hummers' method, which involves hazardous chemicals and is a time-consuming process. In this thesis work, I will introduce a green and feasible process to produce GO and nitrogen-doped GO directly from bio-waste materials without catalyst or substrate. Their applications as oxygen reduction reaction catalyst in fuel cell and fast electroactive actuator will be demonstrated. Then I will explore GO's application in poly(dimethylsiloxane) (PDMS) composites and poly(acrylamide) (PAM) hydrogels. Through interfacial evolution, GO/PDMS composites and GO/PAM hydrogels will be able to stiffen in response to applied cyclic loads. It is shown that the hybrid chemical and physical crosslinking network plays a critical role in the dynamic self-stiffening response. These results provide insight into the complicated nature at the interface between polymer chains and GO, and will help to develop self-stiffening artificial muscle and soft robotics.

Effects of Hydrogel Stiffness and Extracellular Compositions on Modulating Cartilage Regeneration by Mixed Populations of Stem Cells and Chondrocytes In Vivo.

PubMed

Wang, Tianyi; Lai, Janice H; Yang, Fan

2016-12-01

Cell-based therapies offer great promise for repairing cartilage. Previous strategies often involved using a single cell population such as stem cells or chondrocytes. A mixed cell population may offer an alternative strategy for cartilage regeneration while overcoming donor scarcity. We have recently reported that adipose-derived stem cells (ADSCs) can catalyze neocartilage formation by neonatal chondrocytes (NChons) when mixed co-cultured in 3D hydrogels in vitro. However, it remains unknown how the biochemical and mechanical cues of hydrogels modulate cartilage formation by mixed cell populations in vivo. The present study seeks to answer this question by co-encapsulating ADSCs and NChons in 3D hydrogels with tunable stiffness (∼1-33 kPa) and biochemical cues, and evaluating cartilage formation in vivo using a mouse subcutaneous model. Three extracellular matrix molecules were examined, including chondroitin sulfate (CS), hyaluronic acid (HA), and heparan sulfate (HS). Our results showed that the type of biochemical cue played a dominant role in modulating neocartilage deposition. CS and HA enhanced type II collagen deposition, a desirable phenotype for articular cartilage. In contrast, HS promoted fibrocartilage phenotype with the upregulation of type I collagen and failed to retain newly deposited matrix. Hydrogels with stiffnesses of ∼7-33 kPa led to a comparable degree of neocartilage formation, and a minimal initial stiffness was required to retain hydrogel integrity over time. Results from this study highlight the important role of matrix cues in directing neocartilage formation, and they offer valuable insights in guiding optimal scaffold design for cartilage regeneration by using mixed cell populations.

Electro-mechanical properties of hydrogel composites with micro- and nano-cellulose fillers

NASA Astrophysics Data System (ADS)

N, Mohamed Shahid U.; Deshpande, Abhijit P.; Lakshmana Rao, C.

2015-09-01

Stimuli responsive cross-linked hydrogels are of great interest for applications in diverse fields such as sensors and biomaterials. In this study, we investigate polymer composites filled with cellulose fillers. The celluloses used in making the composites were a microcrystalline cellulose of commercial grade and cellulose nano-whiskers obtained through acid hydrolysis of microcrystalline cellulose. The filler concentration was varied and corresponding physical, mechanical and electro-mechanical characterization was carried out. The electro-mechanical properties were determined using a quasi-static method. The fillers not only enhance the mechanical properties of the composite by providing better reinforcement but also provide a quantitative electric potential in the composite. The measurements reveal that the polymer composites prepared from two different cellulose fillers possess a quantitative electric potential which can be utilized in biomedical applications. It is argued that the mechanism behind the quantitative electric potential in the composites is due to streaming potentials arising due to electrical double layer formation.

Glow discharge electrolysis plasma initiated preparation of temperature/pH dual sensitivity reed hemicellulose-based hydrogels.

PubMed

Zhang, Wenming; Zhu, Sha; Bai, Yunping; Xi, Ning; Wang, Shaoyang; Bian, Yang; Li, Xiaowei; Zhang, Yucang

2015-05-20

The temperature/pH dual sensitivity reed hemicellulose-based hydrogels have been prepared through glow discharge electrolysis plasma (GDEP). The effect of different discharge voltages on the temperature and pH response performance of reed hemicellulose-based hydrogels was inspected, and the formation mechanism, deswelling behaviors of reed hemicellulose-based hydrogels were also discussed. At the same time, infrared spectroscopy (FT-IR), scanning differential thermal analysis (DSC) and scanning electron microscope (SEM) were adopted to characterize the structure, phase transformation behaviors and microstructure of hydrogels. It turned out to be that all reed hemicellulose-based hydrogels had a double sensitivity to temperature and pH, and their phase transition temperatures were all approximately 33 °C, as well as the deswelling dynamics met the first model. In addition, the hydrogel (TPRH-3), under discharge voltage 600 V, was more sensitive to temperature and pH and had higher deswelling ratio. Copyright © 2015 Elsevier Ltd. All rights reserved.

Surface-enhanced Raman scattering on molecular self-assembly in nanoparticle-hydrogel composite.

PubMed

Miljanić, Snezana; Frkanec, Leo; Biljan, Tomislav; Meić, Zlatko; Zinić, Mladen

2006-10-24

Surface-enhanced Raman scattering has been applied to study weak intermolecular interactions between small organic gelling molecules involved in the silver nanoparticle-hydrogel composite formation. Assembly and disassembly of the gelator molecules in close vicinity to embedded silver nanoparticles were followed by changes in Raman intensity of the amide II and carboxyl vibrational bands, whereas the strength of the bands related to benzene modes remained constant. This implied that the gelator molecules were strongly attached to the silver particles through the benzene units, while participating in gel structure organization by intermolecular hydrogen bonding between oxalyl amide and carboxyl groups.

Cartilage Repair Using Composites of Human Umbilical Cord Blood-Derived Mesenchymal Stem Cells and Hyaluronic Acid Hydrogel in a Minipig Model.

PubMed

Ha, Chul-Won; Park, Yong-Beom; Chung, Jun-Young; Park, Yong-Geun

2015-09-01

The cartilage regeneration potential of human umbilical cord blood-derived mesenchymal stem cells (hUCB-MSCs) with a hyaluronic acid (HA) hydrogel composite has shown remarkable results in rat and rabbit models. The purpose of the present study was to confirm the consistent regenerative potential in a pig model using three different cell lines. A full-thickness chondral injury was intentionally created in the trochlear groove of each knee in 6 minipigs. Three weeks later, an osteochondral defect, 5 mm wide by 10 mm deep, was created, followed by an 8-mm-wide and 5-mm-deep reaming. A mixture (1.5 ml) of hUCB-MSCs (0.5×10(7) cells per milliliter) and 4% HA hydrogel composite was then transplanted into the defect on the right knee. Each cell line was used in two minipigs. The osteochondral defect created in the same manner on the left knee was untreated to act as the control. At 12 weeks postoperatively, the pigs were sacrificed, and the degree of subsequent cartilage regeneration was evaluated by gross and histological analysis. The transplanted knee resulted in superior and more complete hyaline cartilage regeneration compared with the control knee. The cellular characteristics (e.g., cellular proliferation and chondrogenic differentiation capacity) of the hUCB-MSCs influenced the degree of cartilage regeneration potential. This evidence of consistent cartilage regeneration using composites of hUCB-MSCs and HA hydrogel in a large animal model could be a stepping stone to a human clinical trial in the future. To date, several studies have investigated the chondrogenic potential of human umbilical cord blood-derived mesenchymal stem cells (hUCB-MSCs); however, the preclinical studies are still limited in numbers with various results. In parallel, in the past several years, the cartilage regeneration potential of hUCB-MSCs with a hyaluronic acid (HA) hydrogel composite have been investigated and remarkable results in rat and rabbit models have been attained. (These experimental results are currently in preparation for publication.) Before applying the cartilage regeneration technique in a human clinical trial, it seemed necessary to confirm the consistent result in a larger animal model. At 12 weeks postoperatively, the minipigs were sacrificed, and the degree of subsequent cartilage regeneration was evaluated by gross and histological analysis. The transplanted knee resulted in superior and more complete hyaline cartilage regeneration compared with the control knee. This evidence of consistent cartilage regeneration with composites of hUCB-MSCs and HA hydrogel in a large animal model could be a stepping stone to a human clinical trial in the future. ©AlphaMed Press.

Cartilage Repair Using Composites of Human Umbilical Cord Blood-Derived Mesenchymal Stem Cells and Hyaluronic Acid Hydrogel in a Minipig Model

PubMed Central

Ha, Chul-Won; Chung, Jun-Young; Park, Yong-Geun

2015-01-01

The cartilage regeneration potential of human umbilical cord blood-derived mesenchymal stem cells (hUCB-MSCs) with a hyaluronic acid (HA) hydrogel composite has shown remarkable results in rat and rabbit models. The purpose of the present study was to confirm the consistent regenerative potential in a pig model using three different cell lines. A full-thickness chondral injury was intentionally created in the trochlear groove of each knee in 6 minipigs. Three weeks later, an osteochondral defect, 5 mm wide by 10 mm deep, was created, followed by an 8-mm-wide and 5-mm-deep reaming. A mixture (1.5 ml) of hUCB-MSCs (0.5 × 107 cells per milliliter) and 4% HA hydrogel composite was then transplanted into the defect on the right knee. Each cell line was used in two minipigs. The osteochondral defect created in the same manner on the left knee was untreated to act as the control. At 12 weeks postoperatively, the pigs were sacrificed, and the degree of subsequent cartilage regeneration was evaluated by gross and histological analysis. The transplanted knee resulted in superior and more complete hyaline cartilage regeneration compared with the control knee. The cellular characteristics (e.g., cellular proliferation and chondrogenic differentiation capacity) of the hUCB-MSCs influenced the degree of cartilage regeneration potential. This evidence of consistent cartilage regeneration using composites of hUCB-MSCs and HA hydrogel in a large animal model could be a stepping stone to a human clinical trial in the future. Significance To date, several studies have investigated the chondrogenic potential of human umbilical cord blood-derived mesenchymal stem cells (hUCB-MSCs); however, the preclinical studies are still limited in numbers with various results. In parallel, in the past several years, the cartilage regeneration potential of hUCB-MSCs with a hyaluronic acid (HA) hydrogel composite have been investigated and remarkable results in rat and rabbit models have been attained. (These experimental results are currently in preparation for publication.) Before applying the cartilage regeneration technique in a human clinical trial, it seemed necessary to confirm the consistent result in a larger animal model. At 12 weeks postoperatively, the minipigs were sacrificed, and the degree of subsequent cartilage regeneration was evaluated by gross and histological analysis. The transplanted knee resulted in superior and more complete hyaline cartilage regeneration compared with the control knee. This evidence of consistent cartilage regeneration with composites of hUCB-MSCs and HA hydrogel in a large animal model could be a stepping stone to a human clinical trial in the future. PMID:26240434

Angiogenic potential of gellan-gum-based hydrogels for application in nucleus pulposus regeneration: in vivo study.

PubMed

Silva-Correia, Joana; Miranda-Gonçalves, Vera; Salgado, António J; Sousa, Nuno; Oliveira, Joaquim M; Reis, Rui M; Reis, Rui L

2012-06-01

Hydrogels for nucleus pulposus (NP) regeneration should be able to comprise a nonangiogenic or even antiangiogenic feature. Gellan gum (GG)-based hydrogels have been reported to possess adequate properties for being used as NP substitutes in acellular and cellular strategies, due to its ability to support cell encapsulation, adequate mechanical properties, and noncytotoxicity. In this study, the angiogenic response of GG-based hydrogels was investigated by performing the chorioallantoic membrane assay. The convergence of macroscopic blood vessels toward the GG, ionic-crosslinked methacrylated GG (iGG-MA), and photo-crosslinked methacrylated GG (phGG-MA) hydrogel discs was quantified. Gelatin sponge (GSp) and filter paper (FP) alone and with vascular endothelial growth factor were used as controls of angiogenesis. The images obtained were digitally processed and analyzed by three independent observers. The macroscopic blood vessel quantification demonstrated that the GG-based hydrogels are not angiogenic as compared with FP controls. No statistical differences between the GG-based hydrogels tested in respect to its angiogenic ability were observed. Hematoxylin and eosin staining and SNA-lectin immunohistochemistry assay indicated that the iGG-MA and phGG-MA hydrogels do not allow the ingrowth of chick endothelial cells, following 4 days of implantation. On the contrary, GG, GSp, and FP controls allowed cell infiltration. The histological data also indicated that the GG-based hydrogels do not elicit any acute inflammatory response. The results showed that the GG, iGG-MA, and phGG-MA hydrogels present different permeability to cells but functioned as a physical barrier for vascular invasion. These hydrogels present promising and tunable properties for being used as NP substitutes in the treatment of degenerative intervertebral disc.

Polyelectrolyte hydrogel instabilities in ionic solutions

NASA Astrophysics Data System (ADS)

English, Anthony E.; Tanaka, Toyoichi; Edelman, Elazer R.

1996-12-01

The phase behavior of polyelectrolyte hydrogels has been examined as a function of relative charge composition, bath salt concentration, and solvent quality. Nonlinear swelling instabilities of 2-hydroxyethyl methacrylate (HEMA) and methacrylic acid (MAAc) copolymer hydrogels manifested themselves as discontinuous first order swelling transitions as a function of bath salt concentration. A modified Flory-Huggins model was used to describe the regions of instability when bath salt concentration and solvent quality are considered as control variables. The role of ion dissociation equilibrium in the change from local or smooth transitions to nonlocal or discontinuous swelling transitions is illustrated within the framework of our model.

Biogelx: Cell Culture on Self-Assembling Peptide Gels.

PubMed

Harper, Mhairi M; Connolly, Michael L; Goldie, Laura; Irvine, Eleanore J; Shaw, Joshua E; Jayawarna, Vineetha; Richardson, Stephen M; Dalby, Matthew J; Lightbody, David; Ulijn, Rein V

2018-01-01

Aromatic peptide amphiphiles can form self-supporting nanostructured hydrogels with tunable mechanical properties and chemical compositions. These hydrogels are increasingly applied in two-dimensional (2D) and three-dimensional (3D) cell culture, where there is a rapidly growing need to store, grow, proliferate, and manipulate naturally derived cells within a hydrated, 3D matrix. Biogelx Limited is a biomaterials company, created to commercialize these bio-inspired hydrogels to cell biologists for a range of cell culture applications. This chapter describes methods of various characterization and cell culture techniques specifically optimized for compatibility with Biogelx products.

Synthesis and characterization of GO-hydrogels composites

NASA Astrophysics Data System (ADS)

Pereyra, J. Y.; Cuello, E. A.; Coneo Rodriguez, R.; Barbero, C. A.; Yslas, E. I.; Salavagione, H. J.; Acevedo, D. F.

2017-10-01

The preparation of poly(N-isopropylacrylamide) (PNIPAm) hydrogel nanocomposites containing graphene oxide (GO) and GO plus carbon nanotubes (CNT) in the polymer network is communicated. This one-pot preparation methods include the dispersion of GO (or GO plus CNT) in a solution of monomers and the subsequent polymerization. The texture of the nanocomposites was studied using scanning electron microscopy (SEM), where very compact surfaces are observed suggesting good dispersion of GO sheets and CNTs within the polymer matrix. The presence of GO inside the polymer network diminished the equilibrium swelling values and increased the elastic modulus up to 162 % with respect to the pure gel. Similar results were observed for the composite with CNT. Furthermore, the electrical resistivity of PNIPAm-GO diminishes as the applied compression force increases, being 50 % lower than hydrogel without GO. Moreover, the electrochemical properties of the hydrogels, evaluated by cyclic voltammetry, indicate highly reversible electrical charge/discharge response. In order to apply these materials for antibiotic delivery, the absorption of tetracycline (tet) is evaluated and the nanocomposites showed better absorption capability and improved antibiotic delivery. Preliminary results suggest that tet loaded PNIPAm-GO and PNIPAM-GO-CNT display antimicrobial activity against the Pseudomonas aeruginosa turning these materials as potential candidates for biomedical applications.

Fabricating 3D porous PANI/TiO2-graphene hydrogel for the enhanced UV-light photocatalytic degradation of BPA

NASA Astrophysics Data System (ADS)

Chen, Fangyuan; An, Weijia; Li, Yao; Liang, Yinghua; Cui, Wenquan

2018-01-01

Polyaniline (PANI)/TiO2 composite graphene hydrogel was successfully prepared by chemical reduction method. TiO2 and PANI were uniformly dispersed in the three-dimensional network of graphene hydrogels. This rich network of macroscopic structures not only provides desirable conditions for synergistic adsorption and photocatalytic degradation of pollutants, but also improves the chemical stability of composites. Specifically, 80% PANI/TiO2-reduced graphene oxide hydrogel (rGH) can completely degrade BPA in 40 min, and BPA was almost completely mineralized into small molecules in 65 min. After five cycles of experiments, the degradation rate of PANI/TiO2-rGH for BPA was more than 90%. XPS analysis indicated that there is a strong interaction between PANI and TiO2. Hydrogen bonding between TiO2 and rGH was also demonstrated. Quenching experiments indicated •O2- and h+ are the main active species in the degradation of BPA by PANI/TiO2-rGH and •OH and h+ are the main active species by PANI/TiO2, suggesting that rGH and PANI acts as a transmitter for e- and h+, respectively.

Fibre-reinforced hydrogels for tissue engineering

NASA Astrophysics Data System (ADS)

Waters, Sarah; Byrne, Helen; Chen, Mike; Dias Castilho, Miguel; Kimpton, Laura; Please, Colin; Whiteley, Jonathan

2017-11-01

Tissue engineers aim to grow replacement tissues in vitro to replace those in the body that have been damaged through age, trauma or disease. One approach is to seed cells within a scaffold consisting of an interconnected 3D-printed lattice of polymer fibres, cast in a hydrogel, and subject the construct (cell-seeded scaffold) to an applied load in a bioreactor. A key question is to understand how this applied load is distributed throughout the construct to the mechanosensitive cells. To address this, we exploit the disparate length scales (small inter-fibre spacing compared with construct dimensions). The fibres are treated as a linear elastic material and the hydrogel as a poroelastic material. We employ homogenisation theory to derive equations governing the material properties of a periodic, elastic-poroelastic composite. To validate the mobel, model solutions are compared to experimental data describing the unconfined compression of the fibre-reinforced hydrogels. The model is used to derive the bulk mechanical properties of a cylindrical construct of the composite material for a range of fibre spacings, and the local mechanical environment experienced by cells embedded within the construct is determined. Funded by the European Union Seventh Framework Programme (FP7/2007-2013).

Biomimetic Hydrogel Composites for Soil Stabilization and Contaminant Mitigation.

PubMed

Zhao, Zhi; Hamdan, Nasser; Shen, Li; Nan, Hanqing; Almajed, Abdullah; Kavazanjian, Edward; He, Ximin

2016-11-15

We have developed a novel method to synthesize a hyper-branched biomimetic hydrogel network across a soil matrix to improve the mechanical strength of the loose soil and simultaneously mitigate potential contamination due to excessive ammonium. This method successfully yielded a hierarchical structure that possesses the water retention, ion absorption, and soil aggregation capabilities of plant root systems in a chemically controllable manner. Inspired by the robust organic-inorganic composites found in many living organisms, we have combined this hydrogel network with a calcite biomineralization process to stabilize soil. Our experiments demonstrate that poly(acrylic acid) (PAA) can work synergistically with enzyme-induced carbonate precipitation (EICP) to render a versatile, high-performance soil stabilization method. PAA-enhanced EICP provides multiple benefits including lengthening of water supply time, localization of cementation reactions, reduction of harmful byproduct ammonium, and achievement of ultrahigh soil strength. Soil crusts we have obtained can sustain up to 4.8 × 10 3 kPa pressure, a level comparable to cementitious materials. An ammonium removal rate of 96% has also been achieved. These results demonstrate the potential for hydrogel-assisted EICP to provide effective soil improvement and ammonium mitigation for wind erosion control and other applications.

Hydrogel nanocomposites: a potential UV/blue light filtering material for ophthalmic lenses.

PubMed

Bozukova, Dimitriya; Pagnoulle, Christophe; De Pauw-Gillet, Marie-Claire; Vertruyen, Bénédicte; Jérôme, Robert; Jérôme, Christine

2011-01-01

Poly(2-hydroxyethyl methacrylate-co-methyl methacrylate) (poly(HEMA-co-MMA)) and ZnS hydrogel nanocomposites were prepared and characterized. The chemical composition of the inorganic nanoparticles was confirmed by X-ray diffraction, and the homogeneity of their distribution within the hydrogel was assessed by transmission electron microscopy. The influence of the content of ZnS nanoparticles on the optical performances of the nanocomposites was investigated by UV-Vis spectroscopy. The ability of the hydrogel nanocomposites to filter the hazardous UV light and part of the blue light was reported, which makes them valuable candidates for ophthalmic lens application. In contrast to the optical properties, the thermo-mechanical properties of neat poly(HEMA-co-MMA) hydrogels were found to be largely independent of filling by ZnS nanoparticles (≤2 mg/ml co-monomer mixture). Finally, in vitro cell adhesion test with lens epithelial cells (LECs), extracted from porcine lens crystalline capsule, showed that ZnS had no deleterious effect on the biocompatibility of neat hydrogels, at least at low content. © Koninklijke Brill NV, Leiden, 2011

Protein-based hydrogels for tissue engineering

PubMed Central

Schloss, Ashley C.; Williams, Danielle M.; Regan, Lynne J.

2017-01-01

The tunable mechanical and structural properties of protein-based hydrogels make them excellent scaffolds for tissue engineering and repair. Moreover, using protein-based components provides the option to insert sequences associated with the promoting both cellular adhesion to the substrate and overall cell growth. Protein-based hydrogel components are appealing for their structural designability, specific biological functionality, and stimuli-responsiveness. Here we present highlights in the field of protein-based hydrogels for tissue engineering applications including design requirements, components, and gel types. PMID:27677513

Synthesis of Acylated Xylan-Based Magnetic Fe3O4 Hydrogels and Their Application for H2O2 Detection

PubMed Central

Dai, Qing-Qing; Ren, Jun-Li; Peng, Feng; Chen, Xiao-Feng; Gao, Cun-Dian; Sun, Run-Cang

2016-01-01

Acylated xylan-based magnetic Fe3O4 nanocomposite hydrogels (ACX-MNP-gels) were prepared by fabricating Fe3O4 nanoctahedra in situ within a hydrogel matrix which was synthesized by the copolymerization of acylated xylan (ACX) with acrylamide and N-isopropylacrylamide under ultraviolet irradiation. The size of the Fe3O4 fabricated within the hydrogel matrix could be adjusted through controlling the crosslinking concentrations (C). The magnetic hydrogels showed desirable magnetic and mechanical properties, which were confirmed by XRD, Raman spectroscopy, physical property measurement system, SEM, TGA, and compression test. Moreover, the catalytic performance of the magnetic hydrogels was explored. The magnetic hydrogels (C = 7.5 wt %) presented excellent catalytic activity and provided a sensitive response to H2O2 detection even at a concentration level of 5 × 10−6 mol·L−1. This approach to preparing magnetic hydrogels loaded with Fe3O4 nanoparticles endows xylan-based hydrogels with new promising applications in biotechnology and environmental chemistry. PMID:28773811

Reversible Modulation of DNA-Based Hydrogel Shapes by Internal Stress Interactions.

PubMed

Hu, Yuwei; Kahn, Jason S; Guo, Weiwei; Huang, Fujian; Fadeev, Michael; Harries, Daniel; Willner, Itamar

2016-12-14

We present the assembly of asymmetric two-layer hybrid DNA-based hydrogels revealing stimuli-triggered reversibly modulated shape transitions. Asymmetric, linear hydrogels that include layer-selective switchable stimuli-responsive elements that control the hydrogel stiffness are designed. Trigger-induced stress in one of the layers results in the bending of the linear hybrid structure, thereby minimizing the elastic free energy of the systems. The removal of the stress by a counter-trigger restores the original linear bilayer hydrogel. The stiffness of the DNA hydrogel layers is controlled by thermal, pH (i-motif), K + ion/crown ether (G-quadruplexes), chemical (pH-doped polyaniline), or biocatalytic (glucose oxidase/urease) triggers. A theoretical model relating the experimental bending radius of curvatures of the hydrogels with the Young's moduli and geometrical parameters of the hydrogels is provided. Promising applications of shape-regulated stimuli-responsive asymmetric hydrogels include their use as valves, actuators, sensors, and drug delivery devices.

Biodegradation and Osteosarcoma Cell Cultivation on Poly(aspartic acid) Based Hydrogels.

PubMed

Juriga, Dávid; Nagy, Krisztina; Jedlovszky-Hajdú, Angéla; Perczel-Kovách, Katalin; Chen, Yong Mei; Varga, Gábor; Zrínyi, Miklós

2016-09-14

Development of novel biodegradable and biocompatible scaffold materials with optimal characteristics is important for both preclinical and clinical applications. The aim of the present study was to analyze the biodegradability of poly(aspartic acid)-based hydrogels, and to test their usability as scaffolds for MG-63 osteoblast-like cells. Poly(aspartic acid) was fabricated from poly(succinimide) and hydrogels were prepared using natural amines as cross-linkers (diaminobutane and cystamine). Disulfide bridges were cleaved to thiol groups and the polymer backbone was further modified with RGD sequence. Biodegradability of the hydrogels was evaluated by experiments on the base of enzymes and cell culture medium. Poly(aspartic acid) hydrogels possessing only disulfide bridges as cross-links proved to be degradable by collagenase I. The MG-63 cells showed healthy, fibroblast-like morphology on the double cross-linked and RGD modified hydrogels. Thiolated poly(aspartic acid) based hydrogels provide ideal conditions for adhesion, survival, proliferation, and migration of osteoblast-like cells. The highest viability was found on the thiolated PASP gels while the RGD motif had influence on compacted cluster formation of the cells. These biodegradable and biocompatible poly(aspartic acid)-based hydrogels are promising scaffolds for cell cultivation.

Fibrin hydrogels to deliver dental stem cells of the apical papilla for regenerative medicine.

PubMed

Germain, Loïc; De Berdt, Pauline; Vanacker, Julie; Leprince, Julian; Diogenes, Anibal; Jacobs, Damien; Vandermeulen, Gaëlle; Bouzin, Caroline; Préat, Véronique; Dupont-Gillain, Christine; des Rieux, Anne

2015-01-01

Evaluation of survival, proliferation and neurodifferentiation of dental stem cells from the apical papilla (SCAP) in fibrin hydrogels. We hypothesized that fibrin composition will influence cell behavior. Modulus, pore and fiber size were measured. SCAP in vitro viability, proliferation and neural differentiation, as well as in vivo proliferation and angiogenesis were studied. Hydrogel moduli were influenced by fibrin formulation but not hydrogel morphology, SCAP in vitro viability and proliferation. In total 60% of SCAP expressed PanNeurofilament in vitro without induction in Fibrinogen50-Thrombin10. SCAP proliferated when implanted in vivo and stimulated host endothelial cell infiltration. Fibrinogen30-Thrombin10 or Thrombin50 would be more favorable to in vitro SCAP viability and in vivo proliferation, while Fibrinogen 50-Thrombin50 would be more adapted to neurodifferentiation.

Synthesis, structural characterization and antibacterial activity of cotton fabric modified with a hydrogel containing barium hexaferrite nanoparticles

NASA Astrophysics Data System (ADS)

Staneva, Desislava; Koutzarova, Tatyana; Vertruyen, Benedicte; Vasileva-Tonkova, Evgenia; Grabchev, Ivo

2017-01-01

Barium hexaferrite nanoparticles were synthesized by co-precipitation of Ba2+ and Fe3+ cations with NaOH under of high-power ultrasound. The nanoparticles were dispersed in an aqueous solution of the hydrogel precursors. This solution was used to impregnate the cotton fabric dyed with a photoinitiator. The composite material BaFe12O19 nanoparticles-hydrogel-cotton fabric was prepared by surface initiate photopolymerization under visible light. The modification of the cotton fabric and uniform distribution of the nanoparticles in the structure of the hydrogel were analyzed by scanning electron microscopy (SEM), IR spectroscopy, X-ray diffraction analysis (XRD), fluorescence and colourimetric analyses. The antibacterial efficacy of the material was evaluated against Gram-negative Escherichia coli and Pseudomonas aeruginosa.

Chitosan based hydrogels: characteristics and pharmaceutical applications

PubMed Central

Ahmadi, F.; Oveisi, Z.; Samani, S. Mohammadi; Amoozgar, Z.

2015-01-01

Hydrogel scaffolds serve as semi synthetic or synthetic extra cellular matrix to provide an amenable environment for cellular adherence and cellular remodeling in three dimensional structures mimicking that of natural cellular environment. Additionally, hydrogels have the capacity to carry small molecule drugs and/or proteins, growth factors and other necessary components for cell growth and differentiation. In the context of drug delivery, hydrogels can be utilized to localize drugs, increase drugs concentration at the site of action and consequently reduce off-targeted side effects. The current review aims to describe and classify hydrogels and their methods of production. The main highlight is chitosan-based hydrogels as biocompatible and medically relevant hydrogels for drug delivery. PMID:26430453

Influence of internal composition on physicochemical properties of alginate aqueous-core capsules.

PubMed

Ben Messaoud, Ghazi; Sánchez-González, Laura; Probst, Laurent; Desobry, Stéphane

2016-05-01

To enhance physicochemical properties of alginate aqueous-core capsules, conventional strategies were focused in literature on designing composite and coated capsules. In the present study, own effect of liquid-core composition on mechanical and release properties was investigated. Capsules were prepared by dripping a CaCl2 solution into an alginate gelling solution. Viscosity of CaCl2 solution was adjusted by adding cationic, anionic and non-ionic naturally derived polymers, respectively chitosan, xanthan gum and guar gum. In parallel, uniform alginate hydrogels were prepared by different methods (pouring, in situ forming and mixing). Mechanical stability of capsules and plane hydrogels were respectively evaluated by compression experiments and small amplitude oscillatory shear rheology and then correlated. Capsules permeability was evaluated by monitoring diffusion of encapsulated cochineal dye, riboflavin and BSA. The core-shell interactions were investigated by ATR-FTIR. Results showed that inner polymer had an impact on membrane stability and could act as an internal coating or provide mechanical reinforcement. Mechanical properties of alginate capsules were in a good agreement with rheological behavior of plane hydrogels. Release behavior of the entrapped molecules changed considerably. This study demonstrated the importance of aqueous-core composition, and gave new insights for possible adjusting of microcapsules physicochemical properties by modulating core-shell interactions. Copyright © 2016 Elsevier Inc. All rights reserved.

Development and Characterization of UHMWPE Fiber-Reinforced Hydrogels For Meniscal Replacement

NASA Astrophysics Data System (ADS)

Holloway, Julianne Leigh

Meniscal tears are the most common orthopedic injuries to the human body. The current treatment of choice, however, is a partial meniscectomy that leads to osteoarthritis proportional to the amount of tissue removed. As a result, there is a significant clinical need to develop materials capable of restoring the biomechanical contact stress distribution to the knee after meniscectomy and preventing the onset of osteoarthritis. In this work, a fiber-reinforced hydrogel-based synthetic meniscus was developed that allows for tailoring of the mechanical properties and molding of the implant to match the size, shape, and property distribution of the native tissue. Physically cross-linked poly(vinyl alcohol) (PVA) hydrogels were reinforced with ultrahigh molecular weight polyethylene (UHMWPE) fibers and characterized in compression (0.1-0.8 MPa) and tension (0.1-250 MPa) showing fine control over mechanical properties within the range of the human meniscus. Morphology and crystallinity analysis of PVA hydrogels showed increases in crystallinity and PVA densification, or phase separation, with freeze-thaw cycles. A comparison of freeze-thawed and aged, physically cross-linked hydrogels provided insight on both crystallinity and phase separation as mechanisms for PVA gelation. Results indicated both mechanisms independently contributed to hydrogel modulus for freeze-thawed hydrogels. In vitro swelling studies were performed using osmotic solutions to replicate the swelling pressure present in the knee. Minimal swelling was observed for hydrogels with a PVA concentration of 30-35 wt%, independently of hydrogel freeze-thaw cycles. This allows for independent tailoring of hydrogel modulus and pore structure using freeze-thaw cycles and swelling behavior using polymer concentration to match a wide range of properties needed for various soft tissue applications. The UHMWPE-PVA interface was identified as a significant weakness. To improve interfacial adhesion, a novel biocompatible PVA grafting technique was developed to form a direct covalent linkage at the fiber-matrix interface. Chemical grafting was tailored as a function of the number of sites available for covalent bonding and the percentage of sites reacted. PVA grafting resulted in significant improvements to interfacial shear strength from 11 kPa without any treatment to above 220 kPa following grafting. After grafting, failure was observed cohesively within the PVA hydrogel indicating the UHMWPE-PVA interface was successfully optimized. Lastly, in vitro gait simulations and an in vivo sheep study demonstrated the feasibility and biocompatibility of the proposed UHMWPE-PVA composite. The results from this work can be applied to designing materials for other soft tissue applications, including the anterior cruciate ligament (ACL) and the annulus fibrosus.

Synthesis, characterization, and evaluation of poly(aminoethyl) modified chitosan and its hydrogel used as antibacterial wound dressing.

PubMed

Zhang, Yubei; Dang, Qifeng; Liu, Chengsheng; Yan, Jingquan; Cha, Dongsu; Liang, Shengnan; Li, Xiaoli; Fan, Bing

2017-09-01

This study aims to develop new antibacterial hydrogel wound dressings composed of poly(aminoethyl) modified chitosan (PAEMCS). FTIR, 1 H NMR, and elemental analysis demonstrated that PAEMCS was successfully synthesized via grafting poly(aminoethyl) groups onto hydroxyl groups on chitin first, and removing acetyl groups from the grafted polymer afterward. XRD and TGA implied its well-defined crystallinity and thermostability. Furthermore, a series of hydrogels were fabricated under the participation of dipotassium hydrogen phosphate (DHP). The gelation tests suggested that the higher concentration of PAEMCS or DHP was beneficial to the formation of hydrogels. The pH values of hydrogels at 37°C were all in the range of 7.12-7.50. The rheological tests indicated that PAEMCS-based hydrogels were of lower DHP addition and higher elasticity than CS-based hydrogels to achieve the same gelation temperature under the same polymer's concentration. Additionally, the swelling, anti-bacteria, and cytotoxicity experiments showed that PAEMCS-based hydrogels possessed excellent hygroscopicity, high antibacterial activity against E. coli, S. aureus, or S. epidermidis, and good cytocompatibility toward L929 cells or HUVECs, respectively. All the results implied that PAEMCS-based hydrogels not only maintained inherent multiple properties of chitosan but also possessed excellent antibacterial activity, and might be promising antibacterial hydrogel dressings used in wound therapy. Copyright © 2017 Elsevier B.V. All rights reserved.

Peptide-Modified Zwitterionic Porous Hydrogels for Endothelial Cell and Vascular Engineering

PubMed Central

Lin, Chih-Yeh; Wang, Yi-Ren; Lin, Che-Wei; Wang, Shih-Wen; Chien, Hsiu-Wen; Cheng, Nai-Chen; Tsai, Wei-Bor

2014-01-01

Abstract Hydrogels allow control of gel composition and mechanics, and permit incorporation of cells and a wide variety of molecules from nanoparticles to micromolecules. Peptide-linked hydrogels should tune the basic polymer into a more bioactive template to influence cellular activities. In this study, we first introduced the generation of 2D poly-(sulfobetaine methacrylate [SBMA]) hydrogel surfaces. By incorporating with functional peptide RGD and vascular endothelial growth factor-mimicking peptide KLTWQELYQLKYKG (QK) peptides, endothelial cells attached to the surface well and proliferated in a short-term culturing. However, the mechanical property, which plays a crucial role directing the cellular functions and supporting the structures, decreased when peptides graft onto hydrogels. Manipulating the mechanical property was thus necessary, and the most related factor was the monomer concentration. From our results, the higher amount of SBMA caused greater stiffness in hydrogels. Following the 2D surface studies, we fabricated 3D porous hydrogels for cell scaffolds by several methods. The salt/particle leaching method showed a more reliable way than gas-foaming method to fabricate homogeneous and open-interconnected pores within the hydrogel. Using the salt/particle leaching method, we can control the pore size before leaching. Morphology of endothelial cells within scaffolds was also investigated by scanning electron microscopy, and histological analysis was conducted in vitro and in vivo to test the biocompatibility of SB hydrogel and its potential as a therapeutic reagent for ischemic tissue repair in mice. PMID:25469315

Synthesis and Properties of pH-, Thermo-, and Salt-Sensitive Modified Poly(aspartic acid)/Poly(vinyl alcohol) IPN Hydrogel and Its Drug Controlled Release.

PubMed

Lu, Jingqiong; Li, Yinhui; Hu, Deng; Chen, Xiaoling; Liu, Yongmei; Wang, Liping; Zhao, Yansheng

2015-01-01

Modified poly(aspartic acid)/poly(vinyl alcohol) interpenetrating polymer network (KPAsp/PVA IPN) hydrogel for drug controlled release was synthesized by a simple one-step method in aqueous system using poly(aspartic acid) grafting 3-aminopropyltriethoxysilane (KH-550) and poly(vinyl alcohol) (PVA) as materials. The hydrogel surface morphology and composition were characterized by Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). The thermal stability was analyzed by thermogravimetric analysis (TGA). The swelling properties and pH, temperature, and salt sensitivities of KPAsp, KPAsp/PVA semi-interpenetrating polymer network (semi-IPN), and KPAsp/PVA IPN hydrogels were also investigated. All of the three hydrogels showed ampholytic pH-responsive properties, and swelling behavior was also extremely sensitive to the temperature, ionic strength, and cationic species. Finally, the drug controlled release properties of the three hydrogels were evaluated and results indicated that three hydrogels could control drug release by external surroundings stimuli. The drug controlled release properties of KPAsp/PVA IPN hydrogel are the most outstanding, and the correlative measured release profiles of salicylic acid at 37°C were 32.6 wt% at pH = 1.2 (simulated gastric fluid) and 62.5 wt% at pH = 7.4 (simulated intestinal fluid), respectively. These results indicated that KPAsp/PVA IPN hydrogels are a promising carrier system for controlled drug delivery.

Composite material consisting of microporous β-TCP ceramic and alginate for delayed release of antibiotics.

PubMed

Seidenstuecker, Michael; Ruehe, Juergen; Suedkamp, Norbert P; Serr, Annerose; Wittmer, Annette; Bohner, Marc; Bernstein, Anke; Mayr, Hermann O

2017-03-15

The aim of this study was to produce a novel composite of microporous β-TCP filled with alginate and Vancomycin (VAN) to prolong the release behavior of the antibiotic for up to 28days. Using the flow chamber developed by the group, porous ceramics in a directional flow were filled with alginates of different composition containing 50mg/mL of antibiotics. After cross-linking the alginate with calcium ions, incubation took place in 10mL double-distilled water for 4weeks at 37°C. At defined times (1, 2, 3, 6, 9, 14, 20 and 28days), the liquid was completely exchanged and analyzed by capillary zone electrophoresis and microtiter trials. For statistical purposes, the mean and standard deviation were calculated and analyzed by ANOVA. The release of VAN from alginate was carried out via an external calcium source over the entire period with concentrations above the minimal inhibitory concentration (MIC). The burst release measured 35.2±1.5%. The release of VAN from alginate with an internal calcium source could only be observed over 14days. The burst release here was 61.9±4.3%. The native alginate's burst release was 54.1±7.8%; that of the sterile alginate 40.5±6.4%. The microtiter experiments revealed efficacy over the entire study period for VAN. The MIC value was determined in the release experiments as well in a range of 0.5-2.0μg/mL against Staphylococcus aureus. Drug release systems based on β-TCP and hydrogels are well documented in literature. However, in all described systems the ceramic, as granule or powder, is inserted into a hydrogel. In our work, we do the opposite, a hydrogel which acts as reservoir for antibiotics is placed into a porous biodegradable ceramic. Eventually, this system should be applied as treatment of bone infections. Contrary to the "granule in hydrogel" composites it has the advantage of mechanical stability. Thus, it can take over functions of the bone during the healing process. For a quicker translation from our scientific research into clinical use, only FDA approved materials were used in this work. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Cytocompatible in situ forming chitosan/hyaluronan hydrogels via a metal-free click chemistry for soft tissue engineering.

PubMed

Fan, Ming; Ma, Ye; Mao, Jiahui; Zhang, Ziwei; Tan, Huaping

2015-07-01

Injectable hydrogels are important cell scaffolding materials for tissue engineering and regenerative medicine. Here, we report a new class of biocompatible and biodegradable polysaccharide hydrogels derived from chitosan and hyaluronan via a metal-free click chemistry, without the addition of copper catalyst. For the metal-free click reaction, chitosan and hyaluronan were modified with oxanorbornadiene (OB) and 11-azido-3,6,9-trioxaundecan-1-amine (AA), respectively. The gelation is attributed to the triazole ring formation between OB and azido groups of polysaccharide derivatives. The molecular structures were verified by FT-IR spectroscopy and elemental analysis, giving substitution degrees of 58% and 47% for chitosan-OB and hyaluronan-AA, respectively. The in vitro gelation, morphologies, equilibrium swelling, compressive modulus and degradation of the composite hydrogels were examined. The potential of the metal-free hydrogel as a cell scaffold was demonstrated by encapsulation of human adipose-derived stem cells (ASCs) within the gel matrix in vitro. Cell culture showed that this metal-free hydrogel could support survival and proliferation of ASCs. A preliminary in vivo study demonstrated the usefulness of the hydrogel as an injectable scaffold for adipose tissue engineering. These characteristics provide a potential opportunity to use the metal-free click chemistry in preparation of biocompatible hydrogels for soft tissue engineering applications. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Hydrogel-based three-dimensional cell culture for organ-on-a-chip applications.

PubMed

Lee, Seung Hwan; Shim, Kyu Young; Kim, Bumsang; Sung, Jong Hwan

2017-05-01

Recent studies have reported that three-dimensionally cultured cells have more physiologically relevant functions than two-dimensionally cultured cells. Cells are three-dimensionally surrounded by the extracellular matrix (ECM) in complex in vivo microenvironments and interact with the ECM and neighboring cells. Therefore, replicating the ECM environment is key to the successful cell culture models. Various natural and synthetic hydrogels have been used to mimic ECM environments based on their physical, chemical, and biological characteristics, such as biocompatibility, biodegradability, and biochemical functional groups. Because of these characteristics, hydrogels have been combined with microtechnologies and used in organ-on-a-chip applications to more closely recapitulate the in vivo microenvironment. Therefore, appropriate hydrogels should be selected depending on the cell types and applications. The porosity of the selected hydrogel should be controlled to facilitate the movement of nutrients and oxygen. In this review, we describe various types of hydrogels, external stimulation-based gelation of hydrogels, and control of their porosity. Then, we introduce applications of hydrogels for organ-on-a-chip. Last, we also discuss the challenges of hydrogel-based three-dimensional cell culture techniques and propose future directions. © 2017 American Institute of Chemical Engineers Biotechnol. Prog., 33:580-589, 2017. © 2017 American Institute of Chemical Engineers.

Additive Manufacturing of Catalytically Active Living Materials.

PubMed

Saha, Abhijit; Johnston, Trevor G; Shafranek, Ryan T; Goodman, Cassandra J; Zalatan, Jesse G; Storti, Duane W; Ganter, Mark A; Nelson, Alshakim

2018-04-25

Living materials, which are composites of living cells residing in a polymeric matrix, are designed to utilize the innate functionalities of the cells to address a broad range of applications such as fermentation and biosensing. Herein, we demonstrate the additive manufacturing of catalytically active living materials (AMCALM) for continuous fermentation. A multi-stimuli-responsive yeast-laden hydrogel ink, based on F127-dimethacrylate, was developed and printed using a direct-write 3D printer. The reversible stimuli-responsive behaviors of the polymer hydrogel inks to temperature and pressure are critical, as they enabled the facile incorporation of yeast cells and subsequent fabrication of 3D lattice constructs. Subsequent photo-cross-linking of the printed polymer hydrogel afforded a robust elastic material. These yeast-laden living materials were metabolically active in the fermentation of glucose into ethanol for 2 weeks in a continuous batch process without significant reduction in efficiency (∼90% yield of ethanol). This cell immobilization platform may potentially be applicable toward other genetically modified yeast strains to produce other high-value chemicals in a continuous biofermentation process.

A three-dimensional bioprinting system for use with a hydrogel-based biomaterial and printing parameter characterization.

PubMed

Song, Seung-Joon; Choi, Jaesoon; Park, Yong-Doo; Lee, Jung-Joo; Hong, So Young; Sun, Kyung

2010-11-01

Bioprinting is an emerging technology for constructing tissue or bioartificial organs with complex three-dimensional (3D) structures. It provides high-precision spatial shape forming ability on a larger scale than conventional tissue engineering methods, and simultaneous multiple components composition ability. Bioprinting utilizes a computer-controlled 3D printer mechanism for 3D biological structure construction. To implement minimal pattern width in a hydrogel-based bioprinting system, a study on printing characteristics was performed by varying printer control parameters. The experimental results showed that printing pattern width depends on associated printer control parameters such as printing flow rate, nozzle diameter, and nozzle velocity. The system under development showed acceptable feasibility of potential use for accurate printing pattern implementation in tissue engineering applications and is another example of novel techniques for regenerative medicine based on computer-aided biofabrication system. © 2010, Copyright the Authors. Artificial Organs © 2010, International Center for Artificial Organs and Transplantation and Wiley Periodicals, Inc.

Optical cell separation from three-dimensional environment in photodegradable hydrogels for pure culture techniques.

PubMed

Tamura, Masato; Yanagawa, Fumiki; Sugiura, Shinji; Takagi, Toshiyuki; Sumaru, Kimio; Matsui, Hirofumi; Kanamori, Toshiyuki

2014-05-07

Cell sorting is an essential and efficient experimental tool for the isolation and characterization of target cells. A three-dimensional environment is crucial in determining cell behavior and cell fate in biological analysis. Herein, we have applied photodegradable hydrogels to optical cell separation from a 3D environment using a computer-controlled light irradiation system. The hydrogel is composed of photocleavable tetra-arm polyethylene glycol and gelatin, which optimized cytocompatibility to adjust a composition of crosslinker and gelatin. Local light irradiation could degrade the hydrogel corresponding to the micropattern image designed on a laptop; minimum resolution of photodegradation was estimated at 20 µm. Light irradiation separated an encapsulated fluorescent microbead without any contamination of neighbor beads, even at multiple targets. Upon selective separation of target cells in the hydrogels, the separated cells have grown on another dish, resulting in pure culture. Cell encapsulation, light irradiation and degradation products exhibited negligible cytotoxicity in overall process.

Tuning the Hydration and Lubrication of the Embedded Load-Bearing Hydrogel Fibers.

PubMed

Zhang, Ran; Feng, Yange; Ma, Shuanhong; Cai, Meirong; Yang, Jun; Yu, Bo; Zhou, Feng

2017-03-07

One of the most prominent properties of hydrogels is their excellent hydrolubrication that derives from the strong hydration of the gel network. However, excessive hydration makes hydrogels exhibit a very poor mechanical property, which limits their practical applications. Here, we prepared a novel composite surface of hydrogel nanofibers embedded in an anodic aluminum oxide substrate which exhibited both excellent lubrication and a high load-bearing capacity. Through the copolymerization of acrylic acid and 3-sulfopropyl methacrylate potassium salt, the gel network swelled sufficiently in aqueous solution and caused high osmotic pressure repulsion to bear heavy loads and hence exhibited excellent aqueous lubrication (μ ≈ 0.01). Notably, the friction coefficient of gels showed no dependence on the load in the experiment, whereas it was strongly influenced by the sliding velocity. Additionally, both electrolyte solution and ionic surfactants affect the conformation of the polymer chains, which results in a significant impact on the friction properties of hydrogel fibers.

Sulfobetaine as a zwitterionic mediator for 3D hydroxyapatite mineralization

PubMed Central

Liu, Pingsheng; Song, Jie

2013-01-01

Both positively and negatively charged residues play pivotal roles in recruiting precursor ions or ion clusters, and lowering interfacial energy in natural biomineralization process. Synergistic utilization of opposite charges, however, has rarely been implemented in the design of cytocompatible synthetic scaffolds promoting hydroxyapatite (HA)-mineralization and osteointegration. We report the use of cytocompatible zwitterionic sulfobetaine ligands to enable 3-dimensional in vitro mineralization of HA across covalently crosslinked hydrogels. The overall charge-neutral zwitterionic hydrogel effectively recruited oppositely charged precursor ions while overcame excessive swelling exhibited by anionic and cationic hydrogels under physiological conditions, resulting in denser and structurally well-integrated mineralized composites. Further controls over the size, content, and spatial distribution of the mineral domains within the zwitterionic hydrogel are accomplished by facile adjustments of hydrogel crosslinking densities and the supersaturation rate governing heterogeneous mineral nucleation and growth. These findings should inspire many creative uses of zwitterionic polymers and polymer coatings for skeletal tissue repair and regeneration. PMID:23332320

A Hydrogel of Ultrathin Pure Polyaniline Nanofibers: Oxidant-Templating Preparation and Supercapacitor Application.

PubMed

Zhou, Kun; He, Yuan; Xu, Qingchi; Zhang, Qin'e; Zhou, An'an; Lu, Zihao; Yang, Li-Kun; Jiang, Yuan; Ge, Dongtao; Liu, Xiang Yang; Bai, Hua

2018-05-15

Although challenging, fabrication of porous conducting polymeric materials with excellent electronic properties is crucial for many applications. We developed a fast in situ polymerization approach to pure polyaniline (PANI) hydrogels, with vanadium pentoxide hydrate nanowires as both the oxidant and sacrifice template. A network comprised of ultrathin PANI nanofibers was generated during the in situ polymerization, and the large aspect ratio of these PANI nanofibers allowed the formation of hydrogels at a low solid content of 1.03 wt %. Owing to the ultrathin fibril structure, PANI hydrogels functioning as a supercapacitor electrode display a high specific capacitance of 636 F g -1 , a rate capability, and good cycling stability (∼83% capacitance retention after 10,000 cycles). This method was also extended to the preparation of polypyrrole and poly(3,4-ethylenedioxythiophene) hydrogels. This template polymerization method represents a rational strategy for design of conducing polymer networks, which can be readily integrated in high-performance devices or a further platform for functional composites.

Sulfobetaine as a zwitterionic mediator for 3D hydroxyapatite mineralization.

PubMed

Liu, Pingsheng; Song, Jie

2013-03-01

Both positively and negatively charged residues play pivotal roles in recruiting precursor ions or ion clusters, and lowering interfacial energy in natural biomineralization process. Synergistic utilization of opposite charges, however, has rarely been implemented in the design of cytocompatible synthetic scaffolds promoting hydroxyapatite (HA)-mineralization and osteointegration. We report the use of cytocompatible zwitterionic sulfobetaine ligands to enable 3-dimensional in vitro mineralization of HA across covalently crosslinked hydrogels. The overall charge-neutral zwitterionic hydrogel effectively recruited oppositely charged precursor ions while overcame excessive swelling exhibited by anionic and cationic hydrogels under physiological conditions, resulting in denser and structurally well-integrated mineralized composites. Further controls over the size, content, and spatial distribution of the mineral domains within the zwitterionic hydrogel are accomplished by facile adjustments of hydrogel crosslinking densities and the supersaturation rate governing heterogeneous mineral nucleation and growth. These findings should inspire many creative uses of zwitterionic polymers and polymer coatings for skeletal tissue repair and regeneration. Copyright © 2012 Elsevier Ltd. All rights reserved.

Experimental Investigation of Mechanical and Thermal Properties of Silica Nanoparticle-Reinforced Poly(acrylamide) Nanocomposite Hydrogels

PubMed Central

O’Brien, Victor; Chang, Andrew; Blanco, Matthew; Zabalegui, Aitor; Lee, Hohyun; Asuri, Prashanth

2015-01-01

Current studies investigating properties of nanoparticle-reinforced polymers have shown that nanocomposites often exhibit improved properties compared to neat polymers. However, over two decades of research, using both experimental studies and modeling analyses, has not fully elucidated the mechanistic underpinnings behind these enhancements. Moreover, few studies have focused on developing an understanding among two or more polymer properties affected by incorporation of nanomaterials. In our study, we investigated the elastic and thermal properties of poly(acrylamide) hydrogels containing silica nanoparticles. Both nanoparticle concentration and size affected hydrogel properties, with similar trends in enhancements observed for elastic modulus and thermal diffusivity. We also observed significantly lower swellability for hydrogel nanocomposites relative to neat hydrogels, consistent with previous work suggesting that nanoparticles can mediate pseudo crosslinking within polymer networks. Collectively, these results indicate the ability to develop next-generation composite materials with enhanced mechanical and thermal properties by increasing the average crosslinking density using nanoparticles. PMID:26301505

The influence of matrix properties on growth and morphogenesis of human pancreatic ductal epithelial cells in 3D

PubMed Central

Raza, Asad; Ki, Chang Seok; Lin, Chien-Chi

2013-01-01

A highly tunable synthetic biomimetic hydrogel platform was developed to study the growth and morphogenesis of pancreatic ductal epithelial cells (PDEC) under the influence of a myriad of instructive cues. A PDEC line, PANC-1, was used as a model system to illustrate the importance of matrix compositions on cell fate determination. PANC-1 is an immortalized ductal epithelial cell line widely used in the study of pancreatic tumor cell behaviors. PANC-1 cells are also increasingly explored as a potential cell source for endocrine differentiation. Thus far, most studies related to PANC-1, among other PDEC lines, are performed on 2D culture surfaces. Here, we evaluated the effect of matrix compositions on PANC-1 cell growth and morphogenesis in 3D. Specifically, PANC-1 cells were encapsulated in PEG-based hydrogels prepared by step-growth thiol-ene photopolymerization. It was found that thiol-ene hydrogels provided a cytocompatible environment for encapsulation and 3D culture of PANC-1 cells. In contrast to a monolayer morphology on 2D culture surfaces, PANC-1 cells formed clusters in 3D thiol-ene hydrogels within 4 days of culture. After culturing for 10 days, however, the growth and structures of these clusters were significantly impacted by gel matrix properties, including sensitivity of the matrix to proteases, stiffness of the matrix, and ECM-mimetic motifs. The use of matrix metalloproteinase (MMP) sensitive linker or the immobilization of fibronectin-derived RGDS ligand in the matrix promoted PANC-1 cell growth and encouraged them to adopt ductal cyst-like structures. On the other hand, the encapsulated cells formed smaller and more compact aggregates in non-MMP responsive gels. The incorporation of laminin-derived YIGSR peptide did not enhance cell growth and caused the cells to form compact aggregates. Immobilized YIGSR also enhanced the expression of epithelial cell markers including β-catenin and E-cadherin. These studies have established PEG-peptide hydrogels formed by thiol-ene photo-click reaction as a suitable platform for studying and manipulating pancreatic epithelial cell growth and morphogenesis in 3D. PMID:23602364

Non-monotonic swelling of surface grafted hydrogels induced by pH and/or salt concentration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Longo, Gabriel S.; Department of Biomedical Engineering, Northwestern University, Evanston, Illinois 60208; Chemistry of Life Processes Institute, Northwestern University, Evanston, Illinois 60208

2014-09-28

We use a molecular theory to study the thermodynamics of a weak-polyacid hydrogel film that is chemically grafted to a solid surface. We investigate the response of the material to changes in the pH and salt concentration of the buffer solution. Our results show that the pH-triggered swelling of the hydrogel film has a non-monotonic dependence on the acidity of the bath solution. At most salt concentrations, the thickness of the hydrogel film presents a maximum when the pH of the solution is increased from acidic values. The quantitative details of such swelling behavior, which is not observed when themore » film is physically deposited on the surface, depend on the molecular architecture of the polymer network. This swelling-deswelling transition is the consequence of the complex interplay between the chemical free energy (acid-base equilibrium), the electrostatic repulsions between charged monomers, which are both modulated by the absorption of ions, and the ability of the polymer network to regulate charge and control its volume (molecular organization). In the absence of such competition, for example, for high salt concentrations, the film swells monotonically with increasing pH. A deswelling-swelling transition is similarly predicted as a function of the salt concentration at intermediate pH values. This reentrant behavior, which is due to the coupling between charge regulation and the two opposing effects triggered by salt concentration (screening electrostatic interactions and charging/discharging the acid groups), is similar to that found in end-grafted weak polyelectrolyte layers. Understanding how to control the response of the material to different stimuli, in terms of its molecular structure and local chemical composition, can help the targeted design of applications with extended functionality. We describe the response of the material to an applied pressure and an electric potential. We present profiles that outline the local chemical composition of the hydrogel, which can be useful information when designing applications that pursue or require the absorption of biomolecules or pH-sensitive molecules within different regions of the film.« less

The synthesis and characterization of hydrogel chitosan-alginate with the addition of plasticizer lauric acid for wound dressing application

NASA Astrophysics Data System (ADS)

Izak Rudyardjo, Djony; Wijayanto, Setiawan

2017-05-01

The writers conducted a study about the synthesis and characterization of hydrogel chitosan-alginate by addition plasticizer lauric acid for wound dressing application. The purpose was to find out the impact of lauric acid concentration variation on hydrogel chitosan-alginate to get the best mechanical and physical properties to be applied as wound dressing in accordance with existing standards. This study used commercially chitosan from extract of shells crab, commercially-available alginate from the extract of sargassum sp, and commercial lauric acid from palm starch. The addition of lauric acid was aimed to repair mechanical properties of hydrogel. The composition of chitosan-alginate is 4:1 (v/v), while the lauric acid concentration variations are 0%, 1%, 2%, 3%, 4%, and 5% w/v. The characterization of mechanical properties test (Tensile strength and Elongation at break) at hydrogel showed the hydrogel chitosan-alginate-lauric acid have the characteristic which meets the standard of mechanical properties for human skin. The best performance of hydrogel chitosan-alginate-lauric acid was obtained by increasing luric acid concentration by 4%, which has a thickness value of 125.46±0.63 µm, elongation 28.89±1.01 %, tensile strength (9.01±0.65) MPa, and ability to absorb liquids (601.45 ±1.24) %.

Incorporating simvastatin/poloxamer 407 hydrogel into 3D-printed porous Ti6Al4V scaffolds for the promotion of angiogenesis, osseointegration and bone ingrowth.

PubMed

Liu, Hao; Li, Wei; Liu, Can; Tan, Jie; Wang, Hong; Hai, Bao; Cai, Hong; Leng, Hui-Jie; Liu, Zhong-Jun; Song, Chun-Li

2016-10-27

Three-dimensional porous titanium alloys printed via electron beam melting have low stiffness similar to that of cortical bone and are promising scaffolds for orthopedic applications. However, the bio-inert nature of titanium alloy is poorly compatible with bone ingrowth. We previously observed that simvastatin/poloxamer 407 thermosensitive hydrogel induces endogenous angiogenic/osteogenic growth factors and promotes angiogenesis and osteogenesis, but the mechanical properties of this hydrogel are poor. The purpose of this study was to construct 3D-printed porous titanium scaffolds (pTi scaffolds) filled with simvastatin/hydrogel and evaluate the effects of this composite on osseointegration, bone ingrowth and neovascularization using a tibial defect rabbit model. Four and eight weeks after implantation, the bone volume, bone mineral density, mineral apposition rate, and push-in maximum force of the pTi scaffolds filled with simvastatin/hydrogel were significantly higher than those without simvastatin (p < 0.05). Moreover, filling with simvastatin/hydrogel significantly enhanced vascularization in and around the pTi scaffolds, and a significant correlation was observed between the volume of new bone and neovascularization (p < 0.01). In conclusion, incorporating simvastatin/poloxamer 407 hydrogel into pTi scaffolds significantly improves neovascularization, osseointegration and bone ingrowth.

Evaluation of gelatin-hyaluronic acid composite hydrogels for accelerating wound healing.

PubMed

Wu, Song; Deng, Liang; Hsia, Hanson; Xu, Kai; He, Yu; Huang, Qiangru; Peng, Yi; Zhou, Zhihua; Peng, Cheng

2017-05-01

Excellent wound dressings maintain a warm and moist environment, thus accelerating wound healing. In this study, we cross-linked gelatin and hyaluronic acid with ethyl-3-(3-dimethylaminopropyl) carbodiimide hydrochloride in different ratios (gelatin/hyaluronic acid = 8:2, gelatin/hyaluronic acid = 5:5, gelatin/hyaluronic acid = 2:8), and explored the effects and mechanisms of gelatinhyaluronic acid hydrogels on wound healing. This was done by examining dressing properties, such as fluid uptake ability, water vapor transmission rate, and the rate of water evaporation. We further verified biological function by using in vitro and in vivo wound models. The hydrogels display appropriate fluid uptake ability and good water vapor transmission rate and rate of water evaporation all of which can provide an adequate moisture environment for wound healing. Cell cytotoxicity and proliferation tests show that the hydrogels have no cytotoxicity, furthermore, gelatin/hyaluronic acid = 8:2 hydrogels have the potential to promote cell proliferation. Animal wound models demonstrate that the hydrogels can effectively promote wound healing in vivo, in particular, the gelatin/hyaluronic acid = 8:2 group which promoted the most rapid healing. Accordingly, gelatin-hyaluronic acid dressings, especially the gelatin/hyaluronic acid = 8:2 hydrogels, have a promising outlook for clinical applications in wound healing.

Nanofiber-structured hydrogel yarns with pH-response capacity and cardiomyocyte-drivability for bio-microactuator application.

PubMed

Wu, Shaohua; Duan, Bin; Qin, Xiaohong; Butcher, Jonathan T

2017-09-15

Polymeric hydrogels have great potential in soft biological micro-actuator applications. However, inappropriate micro-architecture, non-anisotropy, weak biomechanics, and inferior response behaviors limit their development. In this study, we designed and manufactured novel polyacrylonitrile (PAN)-based hydrogel yarns composed with uniaxially aligned nanofibers. The nanofibrous hydrogel yarns possessed anisotropic architecture and robust mechanical properties with flexibility, and could be assembled into defined scaffold structures by subsequent processes. The as-prepared hydrogel yarns showed excellent pH response behaviors, with around 100% maximum length and 900% maximum diameter changes, and the pH response was completed within several seconds. Moreover, the hydrogel yarns displayed unique cell-responsive abilities to promote the cell adhesion, proliferation, and smooth muscle differentiation of human adipose derived mesenchymal stem cells (HADMSC). Chicken cardiomyocytes were further seeded onto our nanofibrous hydrogel yarns to engineer living cell-based microactuators. Our results demonstrated that the uniaxially aligned nanofibrous networks within the hydrogel yarns were the key characteristics leading to the anisotropic organization of cardiac cells, and improved sarcomere organization, mimicking the cardiomyocyte bundles in the native myocardium. The construct is capable of sustaining spontaneous cardiomyocyte pumping behaviors for 7days. Our PAN-based nanofibrous hydrogel yarns are attractive for creating linear microactuators with pH-response capacity and biological microactuators with cardiomyocyte-drivability. A mechanically robust polyacrylonitrile-based nanofibrous hydrogel yarn is fabricated by using a modified electrospinning setup in combination with chemical modification processes. The as-prepared hydrogel yarn possesses a uniaxially aligned nanofiber microarchitecture and supports a rapid, pH-dependent expansion/contraction response within a few seconds. Embryonic cardiomyocytes-seeded hydrogel yarn improves the sarcomere organization and mimics the cardiomyocyte bundles in the native myocardium, which sustains spontaneous cardiomyocyte pumping behaviors. The nanofibrous hydrogel yarn has several advantages over traditional bulk hydrogel scaffolds in terms of robust biomechanics, anisotropic aligned architecture, and superior pH response behaviors. Our nanofibrous hydrogel yarn holds the potential to be developed into novel linear and biological microactuators for various biomedical applications. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

On the development of multifunctional luminescent supramolecular hydrogel of gold and egg white

NASA Astrophysics Data System (ADS)

Patra, Sudeshna; Ravulapalli, Sathyavathi; Hahm, Myung Gwan; Tadi, Kiran Kumar; Narayanan, Tharangattu N.

2016-10-01

Highly stable, luminescent, and printable/paintable supramolecular egg white hydrogel-based surface enhanced Raman scattering (SERS) matrix is created by an in situ synthesis of gold clusters inside a luminescent egg white hydrogel (Au-Gel). The synthesis of stable luminescent egg-white-based hydrogel, where the hydrogel can act as a three dimensional (3D) matrix, using a simple cross-linking chemistry, has promising application in the biomedical field including in 3D cell culturing. Furthermore, this functional hydrogel is demonstrated for micromolar-level detection of Rhodamine 6G using the SERS technique, where Au-Gel is painted over a flexible cellulose pad.

Material properties that predict preservative uptake for silicone hydrogel contact lenses.

PubMed

Green, J Angelo; Phillips, K Scott; Hitchins, Victoria M; Lucas, Anne D; Shoff, Megan E; Hutter, Joseph C; Rorer, Eva M; Eydelman, Malvina B

2012-11-01

To assess material properties that affect preservative uptake by silicone hydrogel lenses. We evaluated the water content (using differential scanning calorimetry), effective pore size (using probe penetration), and preservative uptake (using high-performance liquid chromatography with spectrophotometric detection) of silicone and conventional hydrogel soft contact lenses. Lenses grouped similarly based on freezable water content as they did based on total water content. Evaluation of the effective pore size highlighted potential differences between the surface-treated and non-surface-treated materials. The water content of the lens materials and ionic charge are associated with the degree of preservative uptake. The current grouping system for testing contact lens-solution interactions separates all silicone hydrogels from conventional hydrogel contact lenses. However, not all silicone hydrogel lenses interact similarly with the same contact lens solution. Based upon the results of our research, we propose that the same material characteristics used to group conventional hydrogel lenses, water content and ionic charge, can also be used to predict uptake of hydrophilic preservatives for silicone hydrogel lenses. In addition, the hydrophobicity of silicone hydrogel contact lenses, although not investigated here, is a unique contact lens material property that should be evaluated for the uptake of relatively hydrophobic preservatives and tear components.

pH-responsive self-healing injectable hydrogel based on N-carboxyethyl chitosan for hepatocellular carcinoma therapy.

PubMed

Qu, Jin; Zhao, Xin; Ma, Peter X; Guo, Baolin

2017-08-01

Injectable hydrogels with pH-responsiveness and self-healing ability have great potential for anti-cancer drug delivery. Herein, we developed a series of polysaccharide-based self-healing hydrogels with pH-sensitivity as drug delivery vehicles for hepatocellular carcinoma therapy. The hydrogels were prepared by using N-carboxyethyl chitosan (CEC) synthesized via Michael reaction in aqueous solution and dibenzaldehyde-terminated poly(ethylene glycol) (PEGDA). Doxorubicin (Dox), as a model of water-soluble small molecule anti-cancer drug was encapsulated into the hydrogel in situ. Self-healing behavior of the hydrogels was investigated at microscopic and macroscopic levels, and the hydrogels showed rapid self-healing performance without any external stimulus owing to the dynamic covalent Schiff-base linkage between amine groups from CEC and benzaldehyde groups from PEGDA. The chemical structures, rheological property, in vitro gel degradation, morphology, gelation time and in vitro Dox release behavior from the hydrogels were characterized. Injectability was verified by in vitro injection and in vivo subcutaneous injection in a rat. pH-responsive behavior was verified by in vitro Dox release from hydrogels in PBS solutions with different pH values. Furthermore, the activity of Dox released from hydrogel matrix was evaluated by employing human hepatocellular liver carcinoma (HepG2). Cytotoxicity test of the hydrogels using L929 cells confirmed their good cytocompatibility. Together, these pH-responsive self-healing injectable hydrogels are excellent candidates as drug delivery vehicles for liver cancer treatment. STATEMENT OF SIGNIFICANCE: pH-responsive drug delivery system could release drug efficiently in targeted acid environment and minimalize the amount of drug release in normal physiological environment. pH-sensitive injectable hydrogels as smart anti-cancer drug delivery carriers show great potential application for cancer therapy. The hydrogels with self-healing property could prolong their lifetime during implantation and provide the advantage of minimally invasive surgery and high drug-loading ratio. This work reported the design of a series of pH-responsive self-healing injectable hydrogels based on N-carboxyethyl chitosan synthesized in aqueous solution and dibenzaldehyde-terminated poly(ethylene glycol) via a green approach, and demonstrated their potential as intelligent delivery vehicle of doxorubicin for hepatocellular carcinoma therapy via the pH-responsive nature of dynamic Schiff base. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Functional fabrication of recombinant human collagen-phosphorylcholine hydrogels for regenerative medicine applications.

PubMed

Mirazul Islam, M; Cėpla, Vytautas; He, Chaoliang; Edin, Joel; Rakickas, Tomas; Kobuch, Karin; Ruželė, Živilė; Bruce Jackson, W; Rafat, Mehrdad; Lohmann, Chris P; Valiokas, Ramūnas; Griffith, May

2015-01-01

The implant-host interface is a critical element in guiding tissue or organ regeneration. We previously developed hydrogels comprising interpenetrating networks of recombinant human collagen type III and 2-methacryloyloxyethyl phosphorylcholine (RHCIII-MPC) as substitutes for the corneal extracellular matrix that promote endogenous regeneration of corneal tissue. To render them functional for clinical application, we have now optimized their composition and thereby enhanced their mechanical properties. We have demonstrated that such optimized RHCIII-MPC hydrogels are suitable for precision femtosecond laser cutting to produce complementing implants and host surgical beds for subsequent tissue welding. This avoids the tissue damage and inflammation associated with manual surgical techniques, thereby leading to more efficient healing. Although we previously demonstrated in clinical testing that RHCIII-based implants stimulated cornea regeneration in patients, the rate of epithelial cell coverage of the implants needs improvement, e.g. modification of the implant surface. We now show that our 500μm thick RHCIII-MPC constructs comprising over 85% water are suitable for microcontact printing with fibronectin. The resulting fibronectin micropatterns promote cell adhesion, unlike the bare RHCIII-MPC hydrogel. Interestingly, a pattern of 30μm wide fibronectin stripes enhanced cell attachment and showed the highest mitotic rates, an effect that potentially can be utilized for faster integration of the implant. We have therefore shown that laboratory-produced mimics of naturally occurring collagen and phospholipids can be fabricated into robust hydrogels that can be laser profiled and patterned to enhance their potential function as artificial substitutes of donor human corneas. Copyright © 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Multifunctional hybrid networks based on self assembling peptide sequences

NASA Astrophysics Data System (ADS)

Sathaye, Sameer

The overall aim of this dissertation is to achieve a comprehensive correlation between the molecular level changes in primary amino acid sequences of amphiphilic beta-hairpin peptides and their consequent solution-assembly properties and bulk network hydrogel behavior. This has been accomplished using two broad approaches. In the first approach, amino acid substitutions were made to peptide sequence MAX1 such that the hydrophobic surfaces of the folded beta-hairpins from the peptides demonstrate shape specificity in hydrophobic interactions with other beta-hairpins during the assembly process, thereby causing changes to the peptide nanostructure and bulk rheological properties of hydrogels formed from the peptides. Steric lock and key complementary hydrophobic interactions were designed to occur between two beta-hairpin molecules of a single molecule, LNK1 during beta-sheet fibrillar assembly of LNK1. Experimental results from circular dichroism, transmission electron microscopy and oscillatory rheology collectively indicate that the molecular design of the LNK1 peptide can be assigned the cause of the drastically different behavior of the networks relative to MAX1. The results indicate elimination or significant reduction of fibrillar branching due to steric complementarity in LNK1 that does not exist in MAX1, thus supporting the original hypothesis. As an extension of the designed steric lock and key complementarity between two beta-hairpin molecules of the same peptide molecule. LNK1, three new pairs of peptide molecules LP1-KP1, LP2-KP2 and LP3-KP3 that resemble complementary 'wedge' and 'trough' shapes when folded into beta-hairpins were designed and studied. All six peptides individually and when blended with their corresponding shape complement formed fibrillar nanostructures with non-uniform thickness values. Loose packing in the assembled structures was observed in all the new peptides as compared to the uniform tight packing in MAX1 by SANS analysis. This loose packing can be attributed to the designed wedge and trough shapes of the peptides disturbing formation of a uniform bilayer type structure proposed in the case of MAX1 with each hairpin having a flat hydrophobic surface. Although designed changes in hydrophobic shape of the peptide nanofibril core in the new peptides were found to significantly influence the self-assembled nanostructure and network rheological behavior, a lack of direct morphological and rheological evidence to prove shape specific hydrophobic interactions between wedge and trough shaped beta-hairpins was encountered. In the second approach, peptides with established differences in assembly kinetics and bulk mechanical properties of assembled peptide hydrogels were used to develop composite materials with diverse morphological and mechanical properties by blending with the biopolymer hyaluronic acid. The diverse properties of the composites have been correlated to the specific peptide hydrogels used to develop the composite and the different stages of peptide assembly at which blending with hyaluronic acid was carried out. Finally along with overall conclusions, the new area of co-assembly of peptides in solution has been explored and discussed as potential future work following the research discussed in this dissertation. Strategies such as construction of composite hydrogels from blends of MAX1/MAX8 peptide hydrogels and biologically important anionic species such as heparin biopolymer and DNA have been discussed. Another area of future work discussed is the design and study of peptides that can incorporate chemically crosslinkable functional groups in their hydrophobic amino acid side chains that can be covalently crosslinked after peptide assembly into fibrils. Such covalent crosslinking can potentially lead to stiffer individual peptide fibrils due to additional bond formation at the fibrillar core and therefore much stiffer hydrogels due to a synergistic effect. These enhanced stiffness values can render these new hydrogels excellent candidates for applications like development of extracellular mimetic materials and substrates with easily tunable stiffness values for stem cell differentiation studies.

Boron removal by a composite sorbent: Polyethylenimine/tannic acid derivative immobilized in alginate hydrogel beads.

PubMed

Bertagnolli, Caroline; Grishin, Andrey; Vincent, Thierry; Guibal, Eric

2017-03-21

A novel composite material was prepared by the grafting of tannic acid on polyethylenimine (PEI), which allows an efficient sorption of boron (sorption capacity close to 0.89 mmol B g -1 ). The encapsulation of this chelating sorbent (finely crushed) facilitates its use (readily solid/liquid separation, use in fixed-bed columns) at the expense of a loss in sorption capacity (proportionally decreased by the introduction of alginate having poor efficiency for boron uptake). Sorption isotherms are modeled using the Langmuir equation, while the kinetic profiles are presented a good fit by pseudo-second order rate equation. In addition, the encapsulating matrix introduces supplementary resistance to intraparticle diffusion, especially when the resin is dried without control: freeze-drying partially limits this effect. The stability (at long-term storage) of the sorbent is improved when the sorbent is stored under nitrogen atmosphere. The presence of an excess of NaCl was investigated. The degradation of the hydrogel (by ion-exchange of Ca(II) with Na(I)) leads to a decrease in the sorption performance of composite material but the action of Ca(II) ions in the solutions re-stabilizes the hydrogel.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Jie; Viengkham, Malathong; Bertozzi, Carolyn R.

The controlled integration of organic and inorganic components confers natural bone with superior mechanical properties. Bone biogenesis is thought to occur by templated mineralization of hard apatite crystals by an elastic protein scaffold, a process we sought to emulate with synthetic biomimetic hydrogel polymers. Crosslinked polymethacrylamide and polymethacrylate hydrogels were functionalized with mineral-binding ligands and used to template the formation of hydroxyapatite. Strong adhesion between the organic and inorganic materials was achieved for hydrogels functionalized with either carboxylate or hydroxy ligands. The mineral-nucleating potential of hydroxyl groups identified here broadens the design parameters for synthetic bone-like composites and suggests amore » potential role for hydroxylated collagen proteins in bone mineralization.« less

Prodrugs as self-assembled hydrogels: a new paradigm for biomaterials.

PubMed

Vemula, Praveen Kumar; Wiradharma, Nikken; Ankrum, James A; Miranda, Oscar R; John, George; Karp, Jeffrey M

2013-12-01

Prodrug-based self-assembled hydrogels represent a new class of active biomaterials that can be harnessed for medical applications, in particular the design of stimuli responsive drug delivery devices. In this approach, a promoiety is chemically conjugated to a known-drug to generate an amphiphilic prodrug that is capable of forming self-assembled hydrogels. Prodrug-based self-assembled hydrogels are advantageous as they alter the solubility of the drug, enhance drug loading, and eliminate the use of harmful excipients. In addition, self-assembled prodrug hydrogels can be designed to undergo controlled drug release or tailored degradation in response to biological cues. Herein we review the development of prodrug-based self-assembled hydrogels as an emerging class of biomaterials that overcome several common limitations encountered in conventional drug delivery. Published by Elsevier Ltd.

Responsive Hydrogel-based Photonic Nanochains for Microenvironment Sensing and Imaging in Real Time and High Resolution.

PubMed

Luo, Wei; Cui, Qian; Fang, Kai; Chen, Ke; Ma, Huiru; Guan, Jianguo

2018-01-17

Microenvironment sensing and imaging are of importance in microscale zones like microreactors, microfluidic systems, and biological cells. But they are so far implemented only based on chemical colors from dyes or quantum dots, which suffered either from photobleaching, quenching, or photoblinking behaviors, or from limited color gamut. In contrast, structural colors from hydrogel-based photonic crystals (PCs) may be stable and tunable in the whole visible spectrum by diffraction peak shift, facilitating the visual detection with high accuracy. However, the current hydrogel-based PCs are all inappropriate for microscale detection due to the bulk size. Here we demonstrate the smallest hydrogel-based PCs, responsive hydrogel-based photonic nanochains with high-resolution and real-time response, by developing a general hydrogen bond-guided template polymerization method. A variety of mechanically separated stimuli-responsive hydrogel-based photonic nanochains have been obtained in a large scale including those responding to pH, solvent, and temperature. Each of them has a submicrometer diameter and is composed of individual one-dimensional periodic structure of magnetic particles locked by a tens-of-nanometer-thick peapod-like responsive hydrogel shell. Taking the pH-responsive hydrogel-based photonic nanochains, for example, pH-induced hydrogel volume change notably alters the nanochain length, resulting in a significant variation of the structural color. The submicrometer size endows the nanochains with improved resolution and response time by 2-3 orders of magnitude than the previous counterparts. Our results for the first time validate the feasibility of using structural colors for microenvironment sensing and imaging and may further promote the applications of responsive PCs, such as in displays and printing.

A Supramolecular Hydrogel Based on Polyglycerol Dendrimer-Specific Amino Group Recognition.

PubMed

Cho, Ik Sung; Ooya, Tooru

2018-05-24

Dendrimer-based supramolecular hydrogels have gained attention in biomedical fields. While biocompatible dendrimers were used to prepare hydrogels via physical and/or chemical crosslinking, smart functions such as pH and molecular control remain undeveloped. Here, we present polyglycerol dendrimer-based supramolecular hydrogel formation induced by a specific interaction between the polyglycerol dendrimer and an amino group of glycol chitosan. Gelation was achieved by mixing the two aqueous solutions. Hydrogel formation was controlled by varying the polyglycerol dendrimer generation. The hydrogel showed pH-dependent swelling; strongly acidic conditions induced degradation via dissociation of the specific interaction. It also showed unique L-arginine-responsive degradation capability due to competitive exchange of the amino groups of glycol chitosan and L-arginine. These polyglycerol dendrimer-based supramolecular characteristics allow multimodal application in smart biomaterials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Investigation of the surface morphology of biocompatible chitosan-based hydrogels and xerogels

NASA Astrophysics Data System (ADS)

Zhuravleva, Yulia Yu.; Malinkina, Olga N.; Shipovskaya, Anna B.

2018-04-01

Our biocompatible hydrogel systems obtained by the sol-gel technqiue and based on chitosan and silicon polyolates are promising for medical and biological applications. The surface microrelief of these sol-gel materials (hydrogels and xerogels) based on chitosan and silicon tetraglycerolate was explored by AFM and SEM. A significant influence of the component ratio in the mixed system on the morphology and surface profile of the hydrogels and xerogels prepared therefrom was established. An increased content of the structure-forming component (chitosan) in the system was shown to increase the roughness scale of the hydrogel surface and to promote the porosity of the xerogel structure.

Autonomic composite hydrogels by reactive printing: materials and oscillatory response.

PubMed

Kramb, R C; Buskohl, P R; Slone, C; Smith, M L; Vaia, R A

2014-03-07

Autonomic materials are those that automatically respond to a change in environmental conditions, such as temperature or chemical composition. While such materials hold incredible potential for a wide range of uses, their implementation is limited by the small number of fully-developed material systems. To broaden the number of available systems, we have developed a post-functionalization technique where a reactive Ru catalyst ink is printed onto a non-responsive polymer substrate. Using a succinimide-amine coupling reaction, patterns are printed onto co-polymer or biomacromolecular films containing primary amine functionality, such as polyacrylamide (PAAm) or poly-N-isopropyl acrylamide (PNIPAAm) copolymerized with poly-N-(3-Aminopropyl)methacrylamide (PAPMAAm). When the films are placed in the Belousov-Zhabotinsky (BZ) solution medium, the reaction takes place only inside the printed nodes. In comparison to alternative BZ systems, where Ru-containing monomers are copolymerized with base monomers, reactive printing provides facile tuning of a range of hydrogel compositions, as well as enabling the formation of mechanically robust composite monoliths. The autonomic response of the printed nodes is similar for all matrices in the BZ solution concentrations examined, where the period of oscillation decreases in response to increasing sodium bromate or nitric acid concentration. A temperature increase reduces the period of oscillations and temperature gradients are shown to function as pace-makers, dictating the direction of the autonomic response (chemical waves).

A composite scaffold of MSC affinity peptide-modified demineralized bone matrix particles and chitosan hydrogel for cartilage regeneration

NASA Astrophysics Data System (ADS)

Meng, Qingyang; Man, Zhentao; Dai, Linghui; Huang, Hongjie; Zhang, Xin; Hu, Xiaoqing; Shao, Zhenxing; Zhu, Jingxian; Zhang, Jiying; Fu, Xin; Duan, Xiaoning; Ao, Yingfang

2015-12-01

Articular cartilage injury is still a significant challenge because of the poor intrinsic healing potential of cartilage. Stem cell-based tissue engineering is a promising technique for cartilage repair. As cartilage defects are usually irregular in clinical settings, scaffolds with moldability that can fill any shape of cartilage defects and closely integrate with the host cartilage are desirable. In this study, we constructed a composite scaffold combining mesenchymal stem cells (MSCs) E7 affinity peptide-modified demineralized bone matrix (DBM) particles and chitosan (CS) hydrogel for cartilage engineering. This solid-supported composite scaffold exhibited appropriate porosity, which provided a 3D microenvironment that supports cell adhesion and proliferation. Cell proliferation and DNA content analysis indicated that the DBM-E7/CS scaffold promoted better rat bone marrow-derived MSCs (BMMSCs) survival than the CS or DBM/CS groups. Meanwhile, the DBM-E7/CS scaffold increased matrix production and improved chondrogenic differentiation ability of BMMSCs in vitro. Furthermore, after implantation in vivo for four weeks, compared to those in control groups, the regenerated issue in the DBM-E7/CS group exhibited translucent and superior cartilage-like structures, as indicated by gross observation, histological examination, and assessment of matrix staining. Overall, the functional composite scaffold of DBM-E7/CS is a promising option for repairing irregularly shaped cartilage defects.

Subconjunctivally Implanted Hydrogels for Sustained Insulin Release to Reduce Retinal Cell Apoptosis in Diabetic Rats.

PubMed

Imai, Hisanori; Misra, Gauri P; Wu, Linfeng; Janagam, Dileep R; Gardner, Thomas W; Lowe, Tao L

2015-12-01

Diabetic retinopathy (DR) is a leading cause of blindness in diabetic patients that involves early-onset retinal cell loss. Here, we report our recent work using subconjunctivally implantable hydrogels for sustained insulin release to the retina to prevent retinal degeneration. The hydrogels are synthesized by UV photopolymerization of N-isopropylacrylamide and a dextran macromer containing oligolactate-(2-hydroxyetheyl methacrylate) units. Insulin was loaded into the hydrogels during the synthesis. The ex vivo bioactivity of insulin released from the hydrogels was tested on fresh rat retinas using immunoprecipitation and immunoblotting to measure insulin receptor tyrosine and Akt phosphorylation. The biosafety and the effect on the blood glucose of the hydrogels were evaluated in rats 2 months after subconjunctival implantation. The release of insulin from the hydrogels was studied both in vitro in PBS (pH 7.4), and in vivo using confocal microscopy and RIA kit. The in vivo bioactivity of the released insulin was investigated in diabetic rats using DNA fragmentation method. The hydrogels could load insulin with approximately 98% encapsulation efficiency and continuously release FITC-insulin in PBS (pH = 7.4) at 37°C for at least 5 months depending on their composition. Insulin lispro released from the hydrogels was biologically active by increasing insulin receptor tyrosine and Akt serine phosphorylation of ex vivo retinas. In vivo studies showed normal retinal histology 2 months post subconjunctival implantation. Insulin released from subconjunctivally implanted hydrogels could be detected in the retina by using confocal microscopy and RIA kit for 1 week. The implanted hydrogels with insulin lispro did not change the blood glucose level of normal and diabetic rats, but significantly reduced the DNA fragmentation of diabetic retinas for 1 week. The developed hydrogels have great potential to sustain release of insulin to the retina via subconjunctival implantation to minimize DR without the risk of hypoglycemia.

Subconjunctivally Implanted Hydrogels for Sustained Insulin Release to Reduce Retinal Cell Apoptosis in Diabetic Rats

PubMed Central

Imai, Hisanori; Misra, Gauri P.; Wu, Linfeng; Janagam, Dileep R.; Gardner, Thomas W.; Lowe, Tao L.

2015-01-01

Purpose Diabetic retinopathy (DR) is a leading cause of blindness in diabetic patients that involves early-onset retinal cell loss. Here, we report our recent work using subconjunctivally implantable hydrogels for sustained insulin release to the retina to prevent retinal degeneration. Methods The hydrogels are synthesized by UV photopolymerization of N-isopropylacrylamide and a dextran macromer containing oligolactate-(2-hydroxyetheyl methacrylate) units. Insulin was loaded into the hydrogels during the synthesis. The ex vivo bioactivity of insulin released from the hydrogels was tested on fresh rat retinas using immunoprecipitation and immunoblotting to measure insulin receptor tyrosine and Akt phosphorylation. The biosafety and the effect on the blood glucose of the hydrogels were evaluated in rats 2 months after subconjunctival implantation. The release of insulin from the hydrogels was studied both in vitro in PBS (pH 7.4), and in vivo using confocal microscopy and RIA kit. The in vivo bioactivity of the released insulin was investigated in diabetic rats using DNA fragmentation method. Results The hydrogels could load insulin with approximately 98% encapsulation efficiency and continuously release FITC-insulin in PBS (pH = 7.4) at 37°C for at least 5 months depending on their composition. Insulin lispro released from the hydrogels was biologically active by increasing insulin receptor tyrosine and Akt serine phosphorylation of ex vivo retinas. In vivo studies showed normal retinal histology 2 months post subconjunctival implantation. Insulin released from subconjunctivally implanted hydrogels could be detected in the retina by using confocal microscopy and RIA kit for 1 week. The implanted hydrogels with insulin lispro did not change the blood glucose level of normal and diabetic rats, but significantly reduced the DNA fragmentation of diabetic retinas for 1 week. Conclusions The developed hydrogels have great potential to sustain release of insulin to the retina via subconjunctival implantation to minimize DR without the risk of hypoglycemia. PMID:26658505

Poly(vinyl alcohol) hydrogel coatings with tunable surface exposure of hydroxyapatite

PubMed Central

Moreau, David; Villain, Arthur; Ku, David N; Corté, Laurent

2014-01-01

Insufficient bone anchoring is a major limitation of artificial substitutes for connective osteoarticular tissues. The use of coatings containing osseoconductive ceramic particles is one of the actively explored strategies to improve osseointegration and strengthen the bone-implant interface for general tissue engineering. Our hypothesis is that hydroxyapatite (HA) particles can be coated robustly on specific assemblies of PVA hydrogel fibers for the potential anchoring of ligament replacements. A simple dip-coating method is described to produce composite coatings made of microscopic hydroxyapatite (HA) particles dispersed in a poly(vinyl alcohol) (PVA) matrix. The materials are compatible with the requirements for implant Good Manufacturing Practices. They are applied to coat bundles of PVA hydrogel fibers used for the development of ligament implants. By means of optical and electronic microscopy, we show that the coating thickness and surface state can be adjusted by varying the composition of the dipping solution. Quantitative analysis based on backscattered electron microscopy show that the exposure of HA at the coating surface can be tuned from 0 to over 55% by decreasing the weight ratio of PVA over HA from 0.4 to 0.1. Abrasion experiments simulating bone-implant contact illustrate how the coating cohesion and wear resistance increase by increasing the content of PVA relative to HA. Using pullout experiments, we find that these coatings adhere well to the fiber bundles and detach by propagation of a crack inside the coating. These results provide a guide to select coated implants for anchoring artificial ligaments. PMID:25482413

Hydrogel Based Biosensors for In Vitro Diagnostics of Biochemicals, Proteins, and Genes.

PubMed

Jung, Il Young; Kim, Ji Su; Choi, Bo Ram; Lee, Kyuri; Lee, Hyukjin

2017-06-01

Hydrogel-based biosensors have drawn considerable attention due to their various advantages over conventional detection systems. Recent studies have shown that hydrogel biosensors can be excellent alternative systems to detect a wide range of biomolecules, including small biochemicals, pathogenic proteins, and disease specific genes. Due to the excellent physical properties of hydrogels such as the high water content and stimuli-responsive behavior of cross-linked network structures, this system can offer substantial improvement for the design of novel detection systems for various diagnostic applications. The other main advantage of hydrogels is the role of biomimetic three-dimensional (3D) matrix immobilizing enzymes and aptamers within the detection systems, which enhances their stability. This provides ideal reaction conditions for enzymes and aptamers to interact with substrates within the aqueous environment of the hydrogel. In this review, we have highlighted various novel detection approaches utilizing the outstanding properties of the hydrogel. This review summarizes the recent progress of hydrogel-based biosensors and discusses their future perspectives and clinical limitations to overcome. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Dynamic properties of hydrogels and fiber-reinforced hydrogels.

PubMed

Martin, Nicholas; Youssef, George

2018-06-07

Hydrophilic polymers, or hydrogels, are used for a wide variety of biomedical applications, due to their inherent ability to withhold a high-water content. In recent years, a large effort has been focused on tailoring the mechanical properties of these hydrogels to become more appropriate materials for use as anatomical and physiological structural supports. A few of these such methods include using diverse types of polymers, both natural and synthetic, varying the type of molecular cross-linking, as well as combining these efforts to form interpenetrating polymer network hydrogels. While multiple research groups have characterized these various hydrogels under quasi-static conditions, their dynamic properties, representative of native physiological loading scenarios, have been scarcely reported. In this study, an E-glass fiber reinforced family of alginate/PAAm hydrogels cross-linked by both divalent and trivalent cations are fabricated and investigated. The effect of the reinforcement phase on the dynamic and hydration behaviors is then explicated. Additionally, a micromechanics framework for short cylindrical chopped fibers is utilized to discern the contribution of the matrix and fiber constituents on the hydrogel composite. The addition of E-glass fibers resulted in the storage modulus exhibiting a ~50%, 5%, and ~120%, increase with a mere addition of 2 wt% of the reinforcing fibers to Na-, Sr-, and Al-alginate/PAAm, respectively. In studying the cross-linking effect of various divalent (Ba, Ca, Sr) and trivalent (Al, Fe) cations, it was noteworthy that the hydrogels were found to be effective in dissipating energy while resisting mechanical deformation when they are cross-linked with higher molecular weight elements, regardless of valency. This report on the dynamic properties of these hydrogels will help to improve their optimization for future use in biomedical load-bearing applications. Copyright © 2018 Elsevier Ltd. All rights reserved.

Hydrogel films and coatings by swelling-induced gelation

PubMed Central

Moreau, David; Chauvet, Caroline; Etienne, François; Rannou, François P.

2016-01-01

Hydrogel films used as membranes or coatings are essential components of devices interfaced with biological systems. Their design is greatly challenged by the need to find mild synthesis and processing conditions that preserve their biocompatibility and the integrity of encapsulated compounds. Here, we report an approach to produce hydrogel films spontaneously in aqueous polymer solutions. This method uses the solvent depletion created at the surface of swelling polymer substrates to induce the gelation of a thin layer of polymer solution. Using a biocompatible polymer that self-assembles at high concentration [poly(vinyl alcohol)], hydrogel films were produced within minutes to hours with thicknesses ranging from tens to hundreds of micrometers. A simple model and numerical simulations of mass transport during swelling capture the experiments and predict how film growth depends on the solution composition, substrate geometry, and swelling properties. The versatility of the approach was verified with a variety of swelling substrates and hydrogel-forming solutions. We also demonstrate the potential of this technique by incorporating other solutes such as inorganic particles to fabricate ceramic-hydrogel coatings for bone anchoring and cells to fabricate cell-laden membranes for cell culture or tissue engineering. PMID:27821765

Injectable alginate-O-carboxymethyl chitosan/nano fibrin composite hydrogels for adipose tissue engineering.

PubMed

Jaikumar, Dhanya; Sajesh, K M; Soumya, S; Nimal, T R; Chennazhi, K P; Nair, Shantikumar V; Jayakumar, R

2015-03-01

Injectable, biodegradable scaffolds are required for soft tissue reconstruction owing to its minimally invasive approach. Such a scaffold can mimic the native extracellular matrix (ECM), provide uniform distribution of cells and overcome limitations like donor site morbidity, volume loss, etc. So, here we report two classes of biocompatible and biodegradable hydrogel blend systems namely, Alginate/O-carboxymethyl chitosan (O-CMC) and Alginate/poly (vinyl alcohol) (PVA) with the inclusion of fibrin nanoparticles in each. The hydrogels were prepared by ionic cross-linking method. The developed hydrogels were compared in terms of its swelling ratio, degradation profile, compressive strength and elastic moduli. From these preliminary findings, it was concluded that Alginate/O-CMC formed a better blend for tissue engineering applications. The potential of the formed hydrogel as an injectable scaffold was revealed by the survival of adipose derived stem cells (ADSCs) on the scaffold by its adhesion, proliferation and differentiation into adipocytes. Cell differentiation studies of fibrin incorporated hydrogel scaffolds showed better differentiation was confirmed by Oil Red O staining technique. These injectable gels have potential in soft tissue regeneration. Copyright © 2014 Elsevier B.V. All rights reserved.

Extracellular-Matrix-Based and Arg-Gly-Asp–Modified Photopolymerizing Hydrogels for Cartilage Tissue Engineering

PubMed Central

Kim, Hwan D.; Heo, Jiseung; Hwang, Yongsung; Kwak, Seon-Yeong; Park, Ok Kyu; Kim, Hyunbum; Varghese, Shyni

2015-01-01

Articular cartilage damage is a persistent and increasing problem with the aging population. Strategies to achieve complete repair or functional restoration remain a challenge. Photopolymerizing-based hydrogels have long received an attention in the cartilage tissue engineering, due to their unique bioactivities, flexible method of synthesis, range of constituents, and desirable physical characteristics. In the present study, we have introduced unique bioactivity within the photopolymerizing-based hydrogels by copolymerizing polyethylene glycol (PEG) macromers with methacrylated extracellular matrix (ECM) molecules (hyaluronic acid and chondroitin sulfate [CS]) and integrin binding peptides (RGD peptide). Results indicate that cellular morphology, as observed by the actin cytoskeleton structures, was strongly dependent on the type of ECM component as well as the presence of integrin binding moieties. Further, CS-based hydrogel with integrin binding RGD moieties increased the lubricin (or known as superficial zone protein [SZP]) gene expression of the encapsulated chondrocytes. Additionally, CS-based hydrogel displayed cell-responsive degradation and resulted in increased DNA, GAG, and collagen accumulation compared with other hydrogels. This study demonstrates that integrin-mediated interactions within CS microenvironment provide an optimal hydrogel scaffold for cartilage tissue engineering application. PMID:25266634

Safety and efficacy of composite collagen-silver nanoparticle hydrogels as tissue engineering scaffolds

NASA Astrophysics Data System (ADS)

Alarcon, Emilio I.; Udekwu, Klas I.; Noel, Christopher W.; Gagnon, Luke B.-P.; Taylor, Patrick K.; Vulesevic, Branka; Simpson, Madeline J.; Gkotzis, Spyridon; Islam, M. Mirazul; Lee, Chyan-Jang; Richter-Dahlfors, Agneta; Mah, Thien-Fah; Suuronen, Erik J.; Scaiano, Juan C.; Griffith, May

2015-11-01

The increasing number of multidrug resistant bacteria has revitalized interest in seeking alternative sources for controlling bacterial infection. Silver nanoparticles (AgNPs), are amongst the most promising candidates due to their wide microbial spectrum of action. In this work, we report on the safety and efficacy of the incorporation of collagen coated AgNPs into collagen hydrogels for tissue engineering. The resulting hybrid materials at [AgNPs] < 0.4 μM retained the mechanical properties and biocompatibility for primary human skin fibroblasts and keratinocytes of collagen hydrogels; they also displayed remarkable anti-infective properties against S. aureus, S. epidermidis, E. coli and P. aeruginosa at considerably lower concentrations than silver nitrate. Further, subcutaneous implants of materials containing 0.2 μM AgNPs in mice showed a reduction in the levels of IL-6 and other inflammation markers (CCL24, sTNFR-2, and TIMP1). Finally, an analysis of silver contents in implanted mice showed that silver accumulation primarily occurred within the tissue surrounding the implant.The increasing number of multidrug resistant bacteria has revitalized interest in seeking alternative sources for controlling bacterial infection. Silver nanoparticles (AgNPs), are amongst the most promising candidates due to their wide microbial spectrum of action. In this work, we report on the safety and efficacy of the incorporation of collagen coated AgNPs into collagen hydrogels for tissue engineering. The resulting hybrid materials at [AgNPs] < 0.4 μM retained the mechanical properties and biocompatibility for primary human skin fibroblasts and keratinocytes of collagen hydrogels; they also displayed remarkable anti-infective properties against S. aureus, S. epidermidis, E. coli and P. aeruginosa at considerably lower concentrations than silver nitrate. Further, subcutaneous implants of materials containing 0.2 μM AgNPs in mice showed a reduction in the levels of IL-6 and other inflammation markers (CCL24, sTNFR-2, and TIMP1). Finally, an analysis of silver contents in implanted mice showed that silver accumulation primarily occurred within the tissue surrounding the implant. Electronic supplementary information (ESI) available: Representative absorption spectra of AgNP@collagen nanoparticles before and after lyophilization. Absorption spectra for the washes obtained from a 1.0 μM AgNP hydrogel over the course of 5 days. Area under the curve (AUC) calculated from the absorption spectra of 500 μm thickness collagen hydrogels prepared using different concentrations of AgNP@collagen. Selected Cryo-SEM images of BDDGE type I collagen-based hydrogels in the absence or presence of 1.0 μM AgNP. An image of a selected area of a collagen-based hydrogel prepared using AgNO3 instead of AgNP@collagen nanoparticles and Live/Dead staining of human skin fibroblasts taken for 24 hours. Growth inhibition profile for E. coli, S. aureus, S. epidermidis and P. aeruginosa in the presence of hydrogels containing AgNPs. See DOI: 10.1039/c5nr03826j

Engineering three-dimensional cell mechanical microenvironment with hydrogels.

PubMed

Huang, Guoyou; Wang, Lin; Wang, Shuqi; Han, Yulong; Wu, Jinhui; Zhang, Qiancheng; Xu, Feng; Lu, Tian Jian

2012-12-01

Cell mechanical microenvironment (CMM) significantly affects cell behaviors such as spreading, migration, proliferation and differentiation. However, most studies on cell response to mechanical stimulation are based on two-dimensional (2D) planar substrates, which cannot mimic native three-dimensional (3D) CMM. Accumulating evidence has shown that there is a significant difference in cell behavior in 2D and 3D microenvironments. Among the materials used for engineering 3D CMM, hydrogels have gained increasing attention due to their tunable properties (e.g. chemical and mechanical properties). In this paper, we provide an overview of recent advances in engineering hydrogel-based 3D CMM. Effects of mechanical cues (e.g. hydrogel stiffness and externally induced stress/strain in hydrogels) on cell behaviors are described. A variety of approaches to load mechanical stimuli in 3D hydrogel-based constructs are also discussed.

Robust Neurite Extension Following Exogenous Electrical Stimulation within Single Walled Carbon Nanotube-Composite Hydrogels

PubMed Central

Koppes, A. N.; Keating, K. W.; McGregor, A. L.; Koppes, R. A.; Kearns, K. R.; Ziemba, A. M.; McKay, C. A.; Zuidema, J. M.; Rivet, C. J.; Gilbert, R. J.; Thompson, D. M.

2016-01-01

The use of exogenous electrical stimulation to promote nerve regeneration has achieved only limited success. Conditions impeding optimized outgrowth may arise from inadequate stimulus presentation due to differences in injury geometry or signal attenuation. Implantation of an electrically-conductive biomaterial may mitigate this attenuation and provide a more reproducible signal. In this study, a conductive nanofiller (single-walled carbon nanotubes [SWCNT]) was selected as one possible material to manipulate the bulk electrical properties of a collagen type I-10% Matrigel™ composite hydrogel. Neurite outgrowth within hydrogels (SWCNT or nanofiller-free controls) was characterized to determine if: 1) nanofillers influence neurite extension and 2) electrical stimulation of the nanofiller composite hydrogel enhances neurite outgrowth. Increased SWCNT loading (10–100-μg/ml) resulted in greater bulk conductivity (up to 1.7-fold) with no significant changes to elastic modulus. Neurite outgrowth increased 3.3-fold in 20-μg/mL SWCNT loaded biomaterials relative to the nanofiller-free control. Electrical stimulation promoted greater outgrowth (2.9-fold) within SWCNT-free control. The concurrent presentation of electrical stimulation and SWCNT-loaded biomaterials resulted in a 7.0-fold increase in outgrowth relative to the unstimulated, nanofiller-free controls. Local glia residing within the DRG likely contribute, in part, to the observed increases in outgrowth; but it is unknown which specific nanofiller properties influence neurite extension. Characterization of neuronal behavior in model systems, such as those described here, will aid the rational development of biomaterials as well as the appropriate delivery of electrical stimuli to support nerve repair. PMID:27167609

Designer bFGF-incorporated d-form self-assembly peptide nanofiber scaffolds to promote bone repair.

PubMed

He, Bin; Ou, Yunsheng; Chen, Shuo; Zhao, Weikang; Zhou, Ao; Zhao, Jinqiu; Li, Hong; Jiang, Dianming; Zhu, Yong

2017-05-01

d-Form and l-form peptide nanofiber scaffolds can spontaneously form stable β-sheet secondary structures and nanofiber hydrogel scaffolds, and hold some promise in hemostasis and wound healing. We report here on the synthetic self-assembling peptide d-RADA16 and l-RADA16 are both found to produce stable β-sheet secondary structure and nanofiber hydrogel scaffolds based on circular dichroism (CD) spectroscopy, transmission electron microscopy (TEM) and rheology analysis etc. d-RADA16 hydrogel and l-RADA16 hydrogel can enhance obvious bone repair in femoral condyle defects of the Sprague-Dawley (SD) rat model compared to PBS treatment. Based on micro-computed tomography (CT), it was revealed that d-RADA16 hydrogel and l-RADA16 hydrogel were capable to obtain the extensive bone healing. Histological evaluation also found that these two hydrogels facilitate the presence of more mature bone tissue within the femoral condyle defects. Additionally, d-RADA16 hydrogel showed some potential in storing and releasing basic-fibroblast growth factor (bFGF) which was able to further promote bone regeneration based on micro-CT analysis. These results indicate that d-form peptide nanofiber hydrogel have some special capacity for bone repair. Copyright © 2016 Elsevier B.V. All rights reserved.

Impact of RGD amount in dextran-based hydrogels for cell delivery.

PubMed

Riahi, Nesrine; Liberelle, Benoît; Henry, Olivier; De Crescenzo, Gregory

2017-04-01

Dextran is one of the hydrophilic polymers that is used for hydrogel preparation. As any polysaccharide, it presents a high density of hydroxyl groups, which make possible several types of derivatization and crosslinking reactions. Furthermore, dextran is an excellent candidate for hydrogel fabrication with controlled cell/scaffold interactions as it is resistant to protein adsorption and cell adhesion. RGD peptide can be grafted to the dextran in order to promote selected cell adhesion and proliferation. Altogether, we have developed a novel strategy to graft the RGD peptide sequence to dextran-based hydrogel using divinyl sulfone as a linker. The resulting RGD functionalized dextran-based hydrogels were transparent, presented a smooth surface and were easy to handle. The impact of varying RGD peptide amounts, hydrogel porosity and topology upon human umbilical vein endothelial cell (HUVEC) adhesion, proliferation and infiltration was investigated. Our results demonstrated that 0.1% of RGD-modified dextran within the gel was sufficient to support HUVEC cells adhesion to the hydrogel surface. Sodium chloride was added (i) to the original hydrogel mix in order to form a macroporous structure presenting interconnected pores and (ii) to the hydrogel surface to create small orifices essential for cells migration inside the matrix. Copyright © 2017 Elsevier Ltd. All rights reserved.

Cross-Linked Hydrogel for Pharmaceutical Applications: A Review

PubMed Central

2017-01-01

Hydrogels are promising biomaterials because of their important qualities such as biocompatibility, biodegradability, hydrophilicity and non-toxicity. These qualities make hydrogels suitable for application in medical and pharmaceutical field. Recently, a tremendous growth of hydrogel application is seen, especially as gel and patch form, in transdermal drug delivery. This review mainly focuses on the types of hydrogels based on cross-linking and; secondly to describe the possible synthesis methods to design hydrogels for different pharmaceutical applications. The synthesis and chemistry of these hydrogels are discussed using specific pharmaceutical examples. The structure and water content in a typical hydrogel have also been discussed. PMID:29399542

Water-soluble, neutral 3,5-diformyl-BODIPY with extended fluorescence lifetime in a self-healable chitosan hydrogel.

PubMed

Belali, Simin; Emandi, Ganapathi; Cafolla, Atillio A; O'Connell, Barry; Haffner, Benjamin; Möbius, Matthias E; Karimi, Alireza; Senge, Mathias O

2017-11-08

3,5-Diformyl-4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (3,5-diformyl-BODIPY) can be used as an efficient biofunctional cross-linker to generate a new class of chitosan-based hydrogels with fluorescence resonance energy transfer (FRET) dynamics and good solubility in water. The hydrogel was fully characterized by FT-IR, UV-vis, fluorescence, FE-SEM, AFM, rheology and picosecond time-resolved spectroscopic techniques. The self-healing ability was demonstrated by rheological recovery and macroscopic and microscopic observations. The fluorescence lifetime was found to increase in aqueous solution of the BODIPY-chitosan hydrogel compared to the 3,5-diformyl-BODIPY monomer. Calculations based on experimental results such as red-shift and decreased intensity of the emission spectrum of highly dye-concentrated hydrogel in comparison to dilute hydrogels, together with changes in the fluorescence lifetime of the hydrogel at different concentration of dyes, suggest that the BDP-CS hydrogels fluorescence dynamics obey the Förster resonance energy transfer (FRET). Improvements in mechanical and photochemical properties and the acceptable values of BODIPY fluorescence lifetime in the hydrogel matrix indicate the utility of the newly synthesized hydrogels for biomedical applications.

Thermoresponsive, in situ crosslinkable hydrogels based on N-isopropylacrylamide: Fabrication, characterization and mesenchymal stem cell encapsulation

PubMed Central

Klouda, Leda; Perkins, Kevin R.; Watson, Brendan M.; Hacker, Michael C.; Bryant, Stephanie J.; Raphael, Robert M.; Kasper, F. Kurtis; Mikos, Antonios G.

2011-01-01

Hydrogels that solidify in response to a dual, physical and chemical, mechanism upon temperature increase were fabricated and characterized. The hydrogels were based on N-isopropylacrylamide, which renders them thermoresponsive, and contained covalently crosslinkable moieties in the macromers. The effects of the macromer end group, namely acrylate or methacrylate, and the fabrication conditions were investigated on the degradative and swelling properties of the hydrogels. The hydrogels exhibited higher swelling below their lower critical solution temperature (LCST). When immersed in cell culture media at physiological temperature, which was above their LCST, hydrogels showed constant swelling and no degradation over eight weeks, with methacrylated hydrogels having higher swelling than their acrylated analogs. In addition, hydrogels immersed in cell culture media under the same conditions showed lower swelling as compared to phosphate buffered saline. The interplay between chemical crosslinking and thermally induced phase separation affected the swelling characteristics of hydrogels in different media. Mesenchymal stem cells encapsulated in the hydrogels in vitro were viable over three weeks and markers of osteogenic differentiation were detected when the cells were cultured with osteogenic supplements. Hydrogel mineralization in the absence of cells was observed in cell culture medium with the addition of fetal bovine serum and β-glycerol phosphate. The results suggest that these hydrogels may be suitable as carriers for cell delivery in tissue engineering. PMID:21187170

Preparation of Chitosan-based Injectable Hydrogels and Its Application in 3D Cell Culture.

PubMed

Li, Yongsan; Zhang, Yaling; Wei, Yen; Tao, Lei

2017-09-29

The protocol presents a facile, efficient, and versatile method to prepare chitosan-based hydrogels using dynamic imine chemistry. The hydrogel is prepared by mixing solutions of glycol chitosan with a synthesized benzaldehyde terminated polymer gelator, and hydrogels are efficiently obtained in several minutes at room temperature. By varying ratios between glycol chitosan, polymer gelator, and water contents, versatile hydrogels with different gelation times and stiffness are obtained. When damaged, the hydrogel can recover its appearances and modulus, due to the reversibility of the dynamic imine bonds as crosslinkages. This self-healable property enables the hydrogel to be injectable since it can be self-healed from squeezed pieces to an integral bulk hydrogel after the injection process. The hydrogel is also multi-responsive to many bio-active stimuli due to different equilibration statuses of the dynamic imine bonds. This hydrogel was confirmed as bio-compatible, and L929 mouse fibroblast cells were embedded following standard procedures and the cell proliferation was easily assessed by a 3D cell cultivation process. The hydrogel can offer an adjustable platform for different research where a physiological mimic of a 3D environment for cells is profited. Along with its multi-responsive, self-healable, and injectable properties, the hydrogels can potentially be applied as multiple carriers for drugs and cells in future bio-medical applications.

An In Vivo Study of Composite Microgels Based on Hyaluronic Acid and Gelatin for the Reconstruction of Surgically Injured Rat Vocal Folds

ERIC Educational Resources Information Center

Coppoolse, Jiska M. S.; Van Kooten, T. G.; Heris, Hossein K.; Mongeau, Luc; Li, Nicole Y. K.; Thibeault, Susan L.; Pitaro, Jacob; Akinpelu, Olubunm; Daniel, Sam J.

2014-01-01

Purpose: The objective of this study was to investigate local injection with a hierarchically microstructured hyaluronic acid-gelatin (HA-Ge) hydrogel for the treatment of acute vocal fold injury using a rat model. Method: Vocal fold stripping was performed unilaterally in 108 Sprague-Dawley rats. A volume of 25 µl saline (placebo controls),…

Hydrogel microparticles for biosensing

PubMed Central

Le Goff, Gaelle C.; Srinivas, Rathi L.; Hill, W. Adam; Doyle, Patrick S.

2015-01-01

Due to their hydrophilic, biocompatible, and highly tunable nature, hydrogel materials have attracted strong interest in the recent years for numerous biotechnological applications. In particular, their solution-like environment and non-fouling nature in complex biological samples render hydrogels as ideal substrates for biosensing applications. Hydrogel coatings, and later, gel dot surface microarrays, were successfully used in sensitive nucleic acid assays and immunoassays. More recently, new microfabrication techniques for synthesizing encoded particles from hydrogel materials have enabled the development of hydrogel-based suspension arrays. Lithography processes and droplet-based microfluidic techniques enable generation of libraries of particles with unique spectral or graphical codes, for multiplexed sensing in biological samples. In this review, we discuss the key questions arising when designing hydrogel particles dedicated to biosensing. How can the hydrogel material be engineered in order to tune its properties and immobilize bioprobes inside? What are the strategies to fabricate and encode gel particles, and how can particles be processed and decoded after the assay? Finally, we review the bioassays reported so far in the literature that have used hydrogel particle arrays and give an outlook of further developments of the field. PMID:26594056

Poly(ethylene glycol) (PEG)-lactic acid nanocarrier-based degradable hydrogels for restoring the vaginal microenvironment

PubMed Central

Rajan, Sujata Sundara; Turovskiy, Yevgeniy; Singh, Yashveer; Chikindas, Michael L.; Sinko, Patrick J.

2014-01-01

Women with bacterial vaginosis (BV) display reduced vaginal acidity, which make them susceptible to associated infections such as HIV. In the current study, poly(ethylene glycol) (PEG) nanocarrier-based degradable hydrogels were developed for the controlled release of lactic acid in the vagina of BV-infected women. PEG-lactic acid (PEG-LA) nanocarriers were prepared by covalently attaching lactic acid to 8-arm PEG-SH via cleavable thioester bonds. PEG-LA nanocarriers with 4 copies of lactic acid per molecule provided controlled release of lactic acid with a maximum release of 23% and 47% bound lactic acid in phosphate buffered saline (PBS, pH 7.4) and acetate buffer (AB, pH 4.3), respectively. The PEG nanocarrier-based hydrogels were formed by cross-linking the PEG-LA nanocarriers with 4-arm PEG-NHS via degradable thioester bonds. The nanocarrier-based hydrogels formed within 20 min under ambient conditions and exhibited an elastic modulus that was 100-fold higher than the viscous modulus. The nanocarrier-based degradable hydrogels provided controlled release of lactic acid for several hours; however, a maximum release of only 10%–14% bound lactic acid was observed possibly due to steric hindrance of the polymer chains in the cross-linked hydrogel. In contrast, hydrogels with passively entrapped lactic acid showed burst release with complete release within 30 min. Lactic acid showed antimicrobial activity against the primary BV pathogen Gardnerella vaginalis with a minimum inhibitory concentration (MIC) of 3.6 mg/ml. In addition, the hydrogels with passively entrapped lactic acid showed retained antimicrobial activity with complete inhibition G. vaginalis growth within 48 h. The results of the current study collectively demonstrate the potential of PEG nanocarrier-based hydrogels for vaginal administration of lactic acid for preventing and treating BV. PMID:25223229

Reactive hydroxyapatite fillers for pectin biocomposites.

PubMed

Munarin, Fabiola; Petrini, Paola; Barcellona, Giulia; Roversi, Tommaso; Piazza, Laura; Visai, Livia; Tanzi, Maria Cristina

2014-12-01

In this work, a novel injectable biocomposite hydrogel is produced by internal gelation, using pectin as organic matrix and hydroxyapatite either as crosslinking agent and inorganic reinforcement. Tunable gelling kinetics and rheological properties are obtained varying the hydrogels' composition, with the final aim of developing systems for cell immobilization. The reversibility by dissolution of pectin-hydroxyapatite hydrogels is achieved with saline solutions, to possibly accelerate the release of the cells or active agents immobilized. Texture analysis confirms the possibility of extruding the biocomposites from needles with diameters from 20 G to 30 G, indicating that they can be implanted with minimally-invasive approaches, minimizing the pain during injection and the side effects of the open surgery. L929 fibroblasts entrapped in the hydrogels survive to the immobilization procedure and exhibit high cell viability. On the overall, these systems result to be suitable supports for the immobilization of cells for tissue regeneration applications. Copyright © 2014 Elsevier B.V. All rights reserved.

Release mechanisms of acetaminophen from polyethylene oxide/polyethylene glycol matrix tablets utilizing magnetic resonance imaging.

PubMed

Tajiri, Tomokazu; Morita, Shigeaki; Sakamoto, Ryosaku; Suzuki, Masazumi; Yamanashi, Shigeyuki; Ozaki, Yukihiro; Kitamura, Satoshi

2010-08-16

Release mechanism of acetaminophen (AAP) from extended-release tablets of hydrogel polymer matrices containing polyethylene oxide (PEO) and polyethylene glycol (PEG) were achieved using flow-through cell with magnetic resonance imaging (MRI). The hydrogel forming abilities are observed characteristically and the layer thickness which is corresponding to the diffusion length of AAP has a good correlation with the drug release profiles. In addition, polymeric erosion contribution to AAP releasing from hydrogel matrix tablets was directly quantified using size-exclusion chromatography (SEC). The matrix erosion profile indicates that the PEG erosion kinetic depends primarily on the composition ratio of PEG to PEO. The present study has confirmed that the combination of in situ MRI and SEC should be well suited to investigate the drug release mechanisms of hydrogel matrix such as PEO/PEG. Copyright (c) 2010 Elsevier B.V. All rights reserved.

Injectable Hydrogel Scaffold from Decellularized Human Lipoaspirate

PubMed Central

Young, D. Adam; Ibrahim, Dina O.; Hu, Diane; Christman, Karen L.

2010-01-01

Soft tissue fillers are rapidly gaining popularity for aesthetic improvements or repair of adipose tissue deficits. Several injectable biopolymers have been investigated for this purpose but often face rapid resorption or limited adipogenesis, and do not mimic the native adipose extracellular matrix (ECM). We have generated an injectable adipose matrix scaffold by efficiently removing both the cellular and lipid contents of human lipoaspirate. The decellularized material retained a complex composition of peptides and glycosaminoglycans found in native adipose ECM. This matrix can be further processed by solubilizing the extracted ECM to generate a thermally-responsive hydrogel that self-assembles upon subcutaneous injection. This hydrogel also supports the growth and survival of patient matched adipose - derived stem cells in vitro. The development of an injectable hydrogel from human lipoaspirate represents a minimally-invasive option for adipose tissue engineering in terms of both the collection of source material and delivery of the scaffold. PMID:20932943

Narrowing the diversification of supramolecular assemblies by preorganization.

PubMed

Wang, Zhongyan; Liang, Chunhui; Shang, Yuna; He, Shuangshuang; Wang, Ling; Yang, Zhimou

2018-03-13

We designed and synthesized three phosphorylated peptides as precursors of the same peptide Nap-YYY. We found that different precursors led to different materials with almost identical chemical compositions at the final stages. Only Nap-YpYY could form very uniform nanofibers in a stable supramolecular hydrogel by enzyme-instructed self-assembly (EISA) at the physiological temperature (37 °C). In contrast, de-phosphorylation of the other two precursors (Nap-pYYY and Nap-YYpY) resulted in diverse nanostructures in metastable hydrogels with precipitates. The formation of uniform nanomaterials in the stable hydrogels was due to the preorganization property of the precursor Nap-YpYY, which facilitated rapid folding and accelerated the kinetics of hydrogelation of the resulting peptide Nap-YYY generated by the EISA process. Our study demonstrated the importance of the precursor for the self-assembly of nanomaterials and provided a useful strategy to manipulate them.

Biodegradation of PVP-CMC hydrogel film: a useful food packaging material.

PubMed

Roy, Niladri; Saha, Nabanita; Kitano, Takeshi; Saha, Petr

2012-06-20

Hydrogels can offer new opportunities for the design of efficient packaging materials with desirable properties (i.e. durability, biodegradability and mechanical strength). It is a promising and emerging concept, as most of the biopolymer based hydrogels are supposed to be biodegradable, they can be considered as alternative eco-friendly packaging materials. This article reports about synthetic (polyvinylpyrrolidone (PVP)) and biopolymer (carboxymethyl cellulose (CMC)) based a novel hydrogel film and its nature of biodegradability under controlled environmental condition. The dry hydrogel films were prepared by solution casting method and designated as 'PVP-CMC hydrogel films'. The hydrogel film containing PVP and CMC in a ratio of 20:80 shows best mechanical properties among all the test samples (i.e. 10:90, 20:80, 50:50, 80:20 and 90:10). Thus, PVP-CMC hydrogel film of 20:80 was considered as a useful food packaging material and further experiments were carried out with this particular hydrogel film. Biodegradation of the PVP-CMC hydrogel films were studied in liquid state (Czapec-Dox liquid medium+soil extracts) until 8 weeks. Variation in mechanical, viscoelastic properties and weight loss of the hydrogel films with time provide the direct evidence of biodegradation of the hydrogels. About 38% weight loss was observed within 8 weeks. FTIR spectra of the hydrogel films (before and after biodegradation) show shifts of the peaks and also change in the peak intensities, which refer to the physico-chemical change in the hydrogel structure and SEM views of the hydrogels show how internal structure of the PVP-CMC film changes in the course of biodegradation. Copyright © 2012 Elsevier Ltd. All rights reserved.

Hydrogel based QCM aptasensor for detection of avian influenza virus.

PubMed

Wang, Ronghui; Li, Yanbin

2013-04-15

The objective of this study was to develop a quartz crystal microbalance (QCM) aptasensor based on ssDNA crosslinked polymeric hydrogel for rapid, sensitive and specific detection of avian influenza virus (AIV) H5N1. A selected aptamer with high affinity and specificity against AIV H5N1 surface protein was used, and hybridization between the aptamer and ssDNA formed the crosslinker in the polymer hydrogel. The aptamer hydrogel was immobilized on the gold surface of QCM sensor using a self-assembled monolayer method. The hydrogel remained in the state of shrink if no H5N1 virus was present in the sample because of the crosslinking between the aptamer and ssDNA in the polymer network. When it exposed to target virus, the binding reaction between the aptamer and H5N1 virus caused the dissolution of the linkage between the aptamer and ssDNA, resulting in the abrupt swelling of the hydrogel. The swollen hydrogel was monitored by the QCM sensor in terms of decreased frequency. Three polymeric hydrogels with different ratio (100:1 hydrogel I, 10:1 hydrogel II, 1:1 hydrogel III) of acrylamide and the aptamer monomer were synthesized, respectively, and then were used as the QCM sensor coating material. The results showed that the developed hydrogel QCM aptasensor was capable of detecting target H5N1 virus, and among the three developed aptamer hydrogels, hydrogel III coated QCM aptasensor achieved the highest sensitivity with the detection limit of 0.0128 HAU (HA unit). The total detection time from sampling to detection was only 30 min. In comparison with the anti-H5 antibody coated QCM immunosensor, the hydrogel QCM aptasensor lowered the detection limit and reduced the detection time. Copyright © 2012 Elsevier B.V. All rights reserved.

Gelator-polysaccharide hybrid hydrogel for selective and controllable dye release.

PubMed

Li, Ping; Dou, Xiao-Qiu; Tang, Yi-Tian; Zhu, Shenmin; Gu, Jiajun; Feng, Chuan-Liang; Zhang, Di

2012-12-01

In this paper, 1,4-bi(phenylalanine-diglycol)-benzene (PDB) based Low-Molecular-Weight-Gelator (LMWG) hydrogels are modified using hydrophilic polysaccharide (sodium alginate). A set of techniques including Fourier transform infrared (FT-IR) spectroscopy, (1)H Nuclear Magnetic Resonance ((1)H NMR), X-ray powder diffraction (XRD), Ultraviolet-Visible (UV-Vis), and circular dichroism (CD) had confirmed a β-turn arrangement of PDB gelators and a semi-interpenetrating network (semi-IPN), which was formed through hydrogen bonds between LMWG fibers and polysaccharide chains. The evaluation of physicochemical properties of hydrogels indicates that gelator-polysaccharide hybrid hydrogels possess better mechanical and water retention properties than LMWG hydrogels. The release study of dyes (model drug) from both LMWG and hybrid hydrogels was carried out. Compared with PDB based hydrogels, hybrid hydrogels show a selective and controllable release property for certain dyes. The results suggest LMWG-polysaccharide hybrid gels may find potential applications as promising drug delivery vehicles for drug molecules. Copyright © 2012 Elsevier Inc. All rights reserved.

Development and characterization of novel alginate-based hydrogels as vehicles for bone substitutes.

PubMed

Morais, D S; Rodrigues, M A; Silva, T I; Lopes, M A; Santos, M; Santos, J D; Botelho, C M

2013-06-05

In this work three different hydrogels were developed to associate, as vehicles, with the synthetic bone substitute GR-HAP. One based on an alginate matrix (Alg); a second on a mixture of alginate and chitosan (Alg/Ch); and a third on alginate and hyaluronate (Alg/HA), using Ca(2+) ions as cross-linking agents. The hydrogels, as well as the respective injectable bone substitutes (IBSs), were fully characterized from the physical-chemical point of view. Weight change studies proved that all hydrogels were able to swell and degrade within 72 h at pH 7.4 and 4.0, being Alg/HA the hydrogel with the highest degradation rate (80%). Rheology studies demonstrated that all hydrogels are non-Newtonian viscoelastic fluids, and injectability tests showed that IBSs presented low maximum extrusion forces, as well as quite stable average forces. In conclusion, the studied hydrogels present the necessary features to be successfully used as vehicles of GR-HAP, particularly the hydrogel Alg/HA. Copyright © 2013 Elsevier Ltd. All rights reserved.

Light-guiding hydrogels for cell-based sensing and optogenetic synthesis in vivo

NASA Astrophysics Data System (ADS)

Choi, Myunghwan; Choi, Jin Woo; Kim, Seonghoon; Nizamoglu, Sedat; Hahn, Sei Kwang; Yun, Seok Hyun

2013-12-01

Polymer hydrogels are widely used as cell scaffolds for biomedical applications. Although the biochemical and biophysical properties of hydrogels have been investigated extensively, little attention has been paid to their potential photonic functionalities. Here, we report cell-integrated polyethylene glycol-based hydrogels for in vivo optical-sensing and therapy applications. Hydrogel patches containing cells were implanted in awake, freely moving mice for several days and shown to offer long-term transparency, biocompatibility, cell viability and light-guiding properties (loss of <1 dB cm-1). Using optogenetic, glucagon-like peptide-1 secreting cells, we conducted light-controlled therapy using the hydrogel in a mouse model with diabetes and obtained improved glucose homeostasis. Furthermore, real-time optical readout of encapsulated heat-shock-protein-coupled fluorescent reporter cells made it possible to measure the nanotoxicity of cadmium-based bare and shelled quantum dots (CdTe; CdSe/ZnS) in vivo.

Thin Hydrogel Films for Optical Biosensor Applications

PubMed Central

Mateescu, Anca; Wang, Yi; Dostalek, Jakub; Jonas, Ulrich

2012-01-01

Hydrogel materials consisting of water-swollen polymer networks exhibit a large number of specific properties highly attractive for a variety of optical biosensor applications. This properties profile embraces the aqueous swelling medium as the basis of biocompatibility, non-fouling behavior, and being not cell toxic, while providing high optical quality and transparency. The present review focuses on some of the most interesting aspects of surface-attached hydrogel films as active binding matrices in optical biosensors based on surface plasmon resonance and optical waveguide mode spectroscopy. In particular, the chemical nature, specific properties, and applications of such hydrogel surface architectures for highly sensitive affinity biosensors based on evanescent wave optics are discussed. The specific class of responsive hydrogel systems, which can change their physical state in response to externally applied stimuli, have found large interest as sophisticated materials that provide a complex behavior to hydrogel-based sensing devices. PMID:24957962

Hydrogels from Amorphous Calcium Carbonate and Polyacrylic Acid: Bio-Inspired Materials for "Mineral Plastics".

PubMed

Sun, Shengtong; Mao, Li-Bo; Lei, Zhouyue; Yu, Shu-Hong; Cölfen, Helmut

2016-09-19

Given increasing environmental issues due to the large usage of non-biodegradable plastics based on petroleum, new plastic materials, which are economic, environmentally friendly, and recyclable are in high demand. One feasible strategy is the bio-inspired synthesis of mineral-based hybrid materials. Herein we report a facile route for an amorphous CaCO3 (ACC)-based hydrogel consisting of very small ACC nanoparticles physically cross-linked by poly(acrylic acid). The hydrogel is shapeable, stretchable, and self-healable. Upon drying, the hydrogel forms free-standing, rigid, and transparent objects with remarkable mechanical performance. By swelling in water, the material can completely recover the initial hydrogel state. As a matrix, thermochromism can also be easily introduced. The present hybrid hydrogel may represent a new class of plastic materials, the "mineral plastics". © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Development of injectable hydrogels for nucleus pulposus replacement

NASA Astrophysics Data System (ADS)

Thomas, Jonathan D.

Intervertebral disc degeneration has been reported as the underlying cause for 75% of cases of lower back pain and is marked by dehydration of the nucleus pulposus within the intervertebral disc. There have been many implant designs to replace the nucleus pulposus. Some researchers have proposed the replacement of the nucleus pulposus with hydrogel materials. The insertion of devices made from these materials further compromises the annulus of the disc. An ideal nucleus replacement could be injected into the disc space and form a solid in vivo. However, injectable replacements using curing elastomers and thermoplastic materials are not ideal because of the potentially harmful exothermic heat evolved from their reactions and the toxicity of the reactants used. We propose a hydrogel system that can be injected as a liquid at 25°C and solidified to yield a hydrogel within the intervertebral disc at 37°C. In aqueous solutions, these polymers have Lower Critical Solution Temperatures (LCST) between 25-37°C, making them unique candidate materials for this application. Poly(N-isopropylacrylamide) (PNIPAAm) is the most widely studied LCST polymer due to its drastic transition near body temperature. However, by itself, pure PNIPAAm forms a hydrogel that has low water content and can readily undergo plastic deformation. To increase the water content and impart elasticity to PNIPAAm hydrogels, grafted and branched hydrogel systems were created that incorporated the thermogelling PNIPAAm and hydrophilic poly(ethylene glycol) (PEG). In this research, the effects of polymer composition and monomer to initiator ratio, which controls polymer MW, on the in vitro swelling properties (mass, chemical, and compressive mechanical stability) of hydrogels formed from aqueous solutions of these polymers were evaluated. Immersion studies were also conducted in solutions to simulate the osmotic environment of the nucleus pulposus. The effects of repeated compression and unloading cycles on the water content and dimensional recovery of hydrogels made from three candidate polymer formulations were also determined. Unlike PNIPAAm and PEG grafted PNIPAAm hydrogels, PEG branched hydrogels have covalently linked networks. Addition of 7 mol% PEG branches to PNIPAAm resulted in a hydrogel with a higher water content and better elastic recovery than hydrogels made from pure PNIPAAm. PEG branched PNIPAAm hydrogels were shown to have mass, chemical, and compressive mechanical stability in vitro. Furthermore, these hydrogels showed superior dimensional recovery after compressive cycling than pure PNIPAAm and PEG grafted PNIPAAm hydrogels. The 7 mol% PEG branched PNIPAAm hydrogels have suitable swelling and mechanical properties to potentially serve as a nucleus pulposus replacement.

3D printable conducting hydrogels containing chemically converted graphene.

PubMed

Sayyar, Sepidar; Gambhir, Sanjeev; Chung, Johnson; Officer, David L; Wallace, Gordon G

2017-02-02

The development of conducting 3D structured biocompatible scaffolds for the growth of electroresponsive cells is critical in the field of tissue engineering. This work reports the synthesis and 3D processing of UV-crosslinkable conducting cytocompatible hydrogels that are prepared from methacrylated chitosan (ChiMA) containing graphenic nanosheets. The addition of chemically converted graphene resulted in mechanical and electrical properties of the composite that were significantly better than ChiMA itself, as well as improved adhesion, proliferation and spreading of L929 fibroblasts cells. The chemically converted graphene/ChiMA hydrogels were amenable to 3D printing and this was used to produce multilayer scaffolds with enhanced mechanical properties through UV-crosslinking.

Impact of immobilizing of low molecular weight hyaluronic acid within gelatin-based hydrogel through enzymatic reaction on behavior of enclosed endothelial cells.

PubMed

Khanmohammadi, Mehdi; Sakai, Shinji; Taya, Masahito

2017-04-01

The hydrogels having the ability to promote migration and morphogenesis of endothelial cells (ECs) are useful for fabricating vascularized dense tissues in vitro. The present study explores the immobilization of low molecular weight hyaluronic acid (LMWHA) derivative within gelatin-based hydrogel to stimulate migration of ECs. The LMWHA derivative possessing phenolic hydroxyl moieties (LMWHA-Ph) was bound to gelatin-based derivative hydrogel through the horseradish peroxidase-catalyzed reaction. The motility of ECs was analyzed by scratch migration assay and microparticle-based cell migration assay. The incorporated LMWHA-Ph molecules within hydrogel was found to be preserved stably through covalent bonds during incubation. The free and immobilized LMWHA-Ph did not lose an inherent stimulatory effect on human umbilical vein endothelial cells (HUVECs). The immobilized LMWHA-Ph within gelatin-based hydrogel induced the high motility of HUVECs, accompanied by robust cytoskeleton extension, and cell subpopulation expressing CD44 cell receptor. In the presence of immobilized LMWHA-Ph, the migration distance and the number of existing HUVECs were demonstrated to be encouraged in dose-dependent and time-dependent manners. Based on the results obtained in this work, it was concluded that the enzymatic immobilization of LMWHA-Ph within gelatin-based hydrogel represents a promising approach to promote ECs' motility and further exploitation for vascular tissue engineering applications. Copyright © 2017 Elsevier B.V. All rights reserved.

Gellan gum-based hydrogels for intervertebral disc tissue-engineering applications.

PubMed

Silva-Correia, J; Oliveira, J M; Caridade, S G; Oliveira, J T; Sousa, R A; Mano, J F; Reis, R L

2011-06-01

Intervertebral disc (IVD) degeneration is a challenging clinical problem that urgently demands viable nucleus pulposus (NP) implant materials. The best suited biomaterial for NP regeneration has yet to be identified, but it is believed that biodegradable hydrogel-based materials are promising candidates. In this work, we have developed ionic- and photo-crosslinked methacrylated gellan gum (GG-MA) hydrogels to be used in acellular and cellular tissue-engineering strategies for the regeneration of IVDs. The physicochemical properties of the developed hydrogels were investigated by Fourier-transform infrared spectroscopy, (1) H nuclear magnetic resonance and differential scanning calorimetry. The swelling ability and degradation rate of hydrogels were also analysed in phosphate-buffered saline solution at physiological pH for a period of 30 days. Additionally, the morphology and mechanical properties of the hydrogels were assessed under a scanning electron microscope and dynamic compression, respectively. An in vitro study was carried out to screen possible cytotoxicity of the gellan gum-based hydrogels by culturing rat lung fibroblasts (L929 cells) with hydrogel leachables up to 7 days. The results demonstrated that gellan gum was successfully methacrylated. We observed that the produced GG-MA hydrogels possess improved mechanical properties and lower water uptake ability and degradation rate as compared to gellan gum. This work also revealed that GG-MA hydrogels are non-cytotoxic in vitro, thus being promising biomaterials to be used in IVD tissue-engineering strategies. Copyright © 2010 John Wiley & Sons, Ltd.

Sustained Release of Naproxen in a New Kind Delivery System of Carbon Nanotubes Hydrogel

PubMed Central

Peng, Xiahui; Zhuang, Qiang; Peng, Dongming; Dong, Qiuli; Tan, Lini; Jiao, Feipeng; Liu, Linqi; Liu, jingyu; Zhao, Chenxi; Wang, Xiaomei

2013-01-01

In this paper, carbon nanotubes (CNTs) were added into chitosan (CS) hydrogels in the form of chitosan modified CNTs (CS-CNTs) composites to prepare carbon nanotubes hydrogels (CNTs-GEL). The products, named CS-MWCNTs, were characterized by scanning electron microscope (SEM) and Fourier transform infrared (FTIR) spectroscopy. Swelling properties and effect of pH on controlled release performance of the two kinds of hydrogels, CNTs- GEL and pure chitosan hydrogels without CNTs (GEL), were investigated respectively. The results showed that CNTs-GEL possess better controlled release performance than GEL. The releasing equilibrium time of CNTs-GEL was longer than that of GEL in both pH = w7.4 and pH=1.2 conditions, although the release ratios of the model drug are similar in the same pH buffer solutions. It is found that release kinetics is better fitted Ritger-Peppas empirical model indicating a fick-diffusion process in pH = 1.2, while in pH = 7.4 it was non-fick diffusion involving surface diffusion and corrosion diffusion processes. PMID:24523738

Swelling of Superabsorbent Poly(Sodium-Acrylate Acrylamide) Hydrogels and Influence of Chemical Structure on Internally Cured Mortar

NASA Astrophysics Data System (ADS)

Krafcik, Matthew J.; Erk, Kendra A.

Superabsorbent hydrogel particles show promise as internal curing agents for high performance concrete (HPC). These gels can absorb and release large volumes of water and offer a solution to the problem of self-dessication in HPC. However, the gels are sensitive to ions naturally present in concrete. This research connects swelling behavior with gel-ion interactions to optimize hydrogel performance for internal curing, reducing the chance of early-age cracking and increasing the durability of HPC. Four different hydrogels of poly(sodium-acrylate acrylamide) are synthesized and characterized with swelling tests in different salt solutions. Depending on solution pH, ionic character, and gel composition, diffrerent swelling behaviors are observed. As weight percent of acrylic acid increases, gels demonstrate higher swelling ratios in reverse osmosis water, but showed substantially decreased swelling when aqueous cations are present. Additionally, in multivalent cation solutions, overshoot peaks are present, whereby the gels have a peak swelling ratio but then deswell. Multivalent cations interact with deprotonated carboxylic acid groups, constricting the gel and expelling water. Mortar containing hydrogels showed reduced autogenous shrinkage and increased relative humidity.

Genipin cross-linked type II collagen/chondroitin sulfate composite hydrogel-like cell delivery system induces differentiation of adipose-derived stem cells and regenerates degenerated nucleus pulposus.

PubMed

Zhou, Xiaopeng; Wang, Jingkai; Fang, Weijing; Tao, Yiqing; Zhao, Tengfei; Xia, Kaishun; Liang, Chengzhen; Hua, Jianming; Li, Fangcai; Chen, Qixin

2018-04-15

Nucleus pulposus (NP) degeneration is usually the origin of intervertebral disc degeneration and consequent lower back pain. Although adipose-derived stem cell (ADSC)-based therapy is regarded to be promising for the treatment of degenerated NP, there is a lack of viable cell carriers to transplant ADSCs into the NP while maintaining cell function. In this study, we developed a type II collagen/chondroitin sulfate (CS) composite hydrogel-like ADSC (CCSA) delivery system with genipin as the cross-linking agent. The induction effect of the scaffold on ADSC differentiation was studied in vitro, and a rat coccygeal vertebrae degeneration model was used to investigate the regenerative effect of the CCSA system on the degenerated NP in vivo. The results showed that the CCSA delivery system cross-linked with 0.02% genipin was biocompatible and promoted the expressions of NP-specific genes. After the injection of the CCSA system, the disc height, water content, extracellular matrix synthesis, and structure of the degenerated NP were partly restored. Our CCSA delivery system uses minimally invasive approaches to promote the regeneration of degenerated NP and provides an exciting new avenue for the treatment of degenerative disc disease. Nucleus pulposus (NP) degeneration is usually the origin of intervertebral disc degeneration and consequent lower back pain. Stem cell-based tissue engineering is a promising method in NP regeneration, but there is a lack of viable cell carriers to transplant ADSCs into the NP while maintaining cell function. In this study, we developed a type II collagen/chondroitin sulfate (CS) composite hydrogel-like ADSC (CCSA) delivery system with genipin as the cross-linking agent. Although several research groups have studied the fabrication of injectable hydrogel with biological matrix, our study differs from other works. We chose type II collagen and CS, the two primary native components in the NP, as the main materials and combined them according to the natural ratio of collagen and sGAG in the NP. The delivery system is preloaded with ADSCs and can be injected into the NP with a needle, followed by in situ gelation. Genipin is used as a cross-linker to improve the bio-stability of the scaffold, with low cytotoxicity. We investigated the stimulatory effects of our scaffold on the differentiation of ADSCs in vitro and the regenerative effect of the CCSA delivery system on degenerated NP in vivo. Copyright © 2018 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Hydrogels for Hydrophobic Drug Delivery. Classification, Synthesis and Applications

PubMed Central

Stewart, Sarah; Ervine, Michael; Al-Kasasbeh, Rehan; Donnelly, Ryan F.

2018-01-01

Hydrogels have been shown to be very useful in the field of drug delivery due to their high biocompatibility and ability to sustain delivery. Therefore, the tuning of their properties should be the focus of study to optimise their potential. Hydrogels have been generally limited to the delivery of hydrophilic drugs. However, as many of the new drugs coming to market are hydrophobic in nature, new approaches for integrating hydrophobic drugs into hydrogels should be developed. This article discusses the possible new ways to incorporate hydrophobic drugs within hydrogel structures that have been developed through research. This review describes hydrogel-based systems for hydrophobic compound delivery included in the literature. The section covers all the main types of hydrogels, including physical hydrogels and chemical hydrogels. Additionally, reported applications of these hydrogels are described in the subsequent sections. PMID:29364833

Radiation-induced synthesis and swelling properties of p(2-hydroxyethyl methacrylate/itaconic acid/oligo (ethylene glycol) acrylate) terpolymeric hydrogels

NASA Astrophysics Data System (ADS)

Micic, M.; Stamenic, D.; Suljovrujic, E.

2012-09-01

Since it is presumed that by incorporation of pH-responsive (IA) and temperature-responsive (OEGA) co-monomers, it is possible to prepare P(HEMA/IA/OEGA) hydrogels with dual (pH and thermo) responsiveness, the main purpose of our study is to investigate the influence of different mole fractions of IA and especially OEGA on the diversity of the swelling properties of the obtained hydrogels. For that reason, a series of terpolymeric hydrogels with different mole ratios of 2-hydroxyethyl methacrylate (HEMA), itaconic acid (IA) and oligo(ethylene glycol) acrylates (OEGA) was synthesised by gamma radiation. The obtained hydrogels were characterised by swelling studies in the wide pH (2.2-9.0) and temperature range (20-70 °C), confirming dual (pH and thermo) responsiveness and a large variation in the swelling capability. It was observed that the equilibrium swelling of P(HEMA/IA/OEGA) hydrogels, for a constant amount of IA, increased progressively with an increase in OEGA share. On the other hand, the dissociation of carboxyl groups from IA occurs at pH>4; therefore, small mole fractions of IA render good pH sensitivity and a large increase in the swelling capacity of these hydrogels at higher pH values. Additional characterisation of structure and properties was conducted by Fourier transform infrared (FTIR) spectroscopy, scanning electron microscopy (SEM) and mechanical measurements, confirming that the inherent properties of P(HEMA/IA/OEGA) hydrogels can be significantly tuned by variation in their composition. According to all presented, it seems that the obtained hydrogels can be a beneficial synergetic combination for controlled delivery of bioactive molecules such as drugs, peptides, proteins, etc.

Gellan Gum-Based Hydrogels for Osteochondral Repair.

PubMed

Costa, Lígia; Silva-Correia, Joana; Oliveira, J Miguel; Reis, Rui L

2018-01-01

Gellan gum (GG) is a widely explored natural polysaccharide that has been gaining attention in tissue engineering (TE) and regenerative medicine field, and more recently in osteochondral TE approaches. Taking advantage of its inherent features such as biocompatibility, biodegradability, similarity with the extracellular matrix and easy functionalization, GG-based hydrogels have been studied for their potential for cartilage and bone tissue regeneration. Several preclinical studies describe the successful outcome of GG in cartilage tissue engineering. By its turn, GG composites have also been proposed in several strategies to guide bone formation. The big challenge in osteochondral TE approaches is still to achieve cartilage and bone regeneration simultaneously through a unique integrated bifunctional construct. The potential of GG to be used as polymeric support to reach both bone and cartilage regeneration has been demonstrated. This chapter provides an overview of GG properties and the functionalization strategies employed to tailor its behaviour to a particular application. The use of GG in soft and hard tissues regeneration approaches, as well in osteochondral integrated TE strategies is also revised.

Reinforcement Strategies for Load-Bearing Calcium Phosphate Biocements

PubMed Central

Geffers, Martha; Groll, Jürgen; Gbureck, Uwe

2015-01-01

Calcium phosphate biocements based on calcium phosphate chemistry are well-established biomaterials for the repair of non-load bearing bone defects due to the brittle nature and low flexural strength of such cements. This article features reinforcement strategies of biocements based on various intrinsic or extrinsic material modifications to improve their strength and toughness. Altering particle size distribution in conjunction with using liquefiers reduces the amount of cement liquid necessary for cement paste preparation. This in turn decreases cement porosity and increases the mechanical performance, but does not change the brittle nature of the cements. The use of fibers may lead to a reinforcement of the matrix with a toughness increase of up to two orders of magnitude, but restricts at the same time cement injection for minimal invasive application techniques. A novel promising approach is the concept of dual-setting cements, in which a second hydrogel phase is simultaneously formed during setting, leading to more ductile cement–hydrogel composites with largely unaffected application properties.

In vitro BMP-2 peptide release from thiolated chitosan based hydrogel.

PubMed

Liu, Xujie; Yu, Bo; Huang, Qianli; Liu, Rui; Feng, Qingling; Cai, Qiang; Mi, Shengli

2016-12-01

Thiolated chitosan based thermo-sensitive hydrogel is a water soluble system and the existing thiol groups are beneficial for the delivery of cysteine-rich peptides. In the present study, a kind of thiolated chitosan, i.e. chitosan-4-thio-butylamidine (CS-TBA) conjugate was characterized and used to prepare CS-TBA/hydroxyapatite (HA)/beta-glycerophosphate disodium (β-GP) thermo-sensitive hydrogel. The cysteine terminated peptide 24 (P24) containing residues 73-92 of the knuckle epitope of BMP-2 (N→C: KIPKASSVPTELSAISTLYLSGGC) was synthesized and characterized. The release behavior of P24 from CS-TBA based hydrogel was investigated in vitro. The thiol groups in CS-TBA may react with thiol groups in P24, thus decreases the P24 release rate and maintains the peptide release for a longer time compared with unmodified chitosan based hydrogel. Moreover, the bioactivity of P24 is preserved during release process. These results indicate that P24 loaded CS-TBA based thermosensitive hydrogel is a potential material for minimally invasive surgery of bone repair. Copyright © 2016 Elsevier B.V. All rights reserved.

Hydrogel-Based Drug Delivery Systems for Poorly Water-Soluble Drugs.

PubMed

McKenzie, Matthew; Betts, David; Suh, Amy; Bui, Kathryn; Kim, London Doyoung; Cho, Hyunah

2015-11-13

Hydrogels are three-dimensional materials that can withstand a great amount of water incorporation while maintaining integrity. This allows hydrogels to be very unique biomedical materials, especially for drug delivery. Much effort has been made to incorporate hydrophilic molecules in hydrogels in the field of drug delivery, while loading of hydrophobic drugs has not been vastly studied. However, in recent years, research has also been conducted on incorporating hydrophobic molecules within hydrogel matrices for achieving a steady release of drugs to treat various ailments. Here, we summarize the types of hydrogels used as drug delivery vehicles, various methods to incorporate hydrophobic molecules in hydrogel matrices, and the potential therapeutic applications of hydrogels in cancer.

Formulation and evaluation of microemulsion-based hydrogel for topical delivery.

PubMed

Sabale, Vidya; Vora, Sejal

2012-07-01

The purpose of this study was to develop microemulsion-based hydrogel formulation for topical delivery of bifonazole with an objective to increase the solubility and skin permeability of the drug. Oleic acid was screened as the oil phase of microemulsions, due to a good solubilizing capacity of the microemulison systems. The pseudo-ternary phase diagrams for microemulsion regions were constructed using oleic acid as the oil, Tween 80 as the surfactant and isopropyl alcohol (IPA) as the cosurfactant. Various microemulsion formulations were prepared and optimized by 3(2) factorial design on the basis of percentage (%) transmittance, globule size, zeta potential, drug release, and skin permeability. The abilities of various microemulsions to deliver bifonazole through the skin were evaluated ex vivo using Franz diffusion cells fitted with rat skins. The Hydroxy Propyl Methyl Cellulose (HPMC) K100 M as a gel matrix was used to construct the microemulsion-based hydrogel for improving the viscosity of microemulsion for topical administration. The optimized microemulsion-based hydrogel was evaluated for viscosity, spreadability, skin irritancy, skin permeability, stability, and antifungal activity by comparing it with marketed bifonazole cream. The mechanism of drug release from microemulsion-based hydrogel was observed to follow zero order kinetics. The studied optimized microemulsion-based hydrogel showed a good stability over the period of 3 months. Average globule size of optimized microemulsion (F5) was found to be 18.98 nm, zeta potential was found to be -5.56 mv, and permeability of drug from microemulsion within 8 h was observed 84%. The antifungal activity of microemulsion-based hydrogel was found to be comparable with marketed cream. The results indicate that the studied microemulsion-based hydrogel (F5) has a potential for sustained action of drug release and it may act as promising vehicle for topical delivery of ibuprofen.

Development of Poly(Ethylene Glycol) Hydrogels for Salivary Gland Tissue Engineering Applications

PubMed Central

Shubin, Andrew D.; Felong, Timothy J.; Graunke, Dean; Ovitt, Catherine E.

2015-01-01

More than 40,000 patients are diagnosed with head and neck cancers annually in the United States with the vast majority receiving radiation therapy. Salivary glands are irreparably damaged by radiation therapy resulting in xerostomia, which severely affects patient quality of life. Cell-based therapies have shown some promise in mouse models of radiation-induced xerostomia, but they suffer from insufficient and inconsistent gland regeneration and accompanying secretory function. To aid in the development of regenerative therapies, poly(ethylene glycol) hydrogels were investigated for the encapsulation of primary submandibular gland (SMG) cells for tissue engineering applications. Different methods of hydrogel formation and cell preparation were examined to identify cytocompatible encapsulation conditions for SMG cells. Cell viability was much higher after thiol-ene polymerizations compared with conventional methacrylate polymerizations due to reduced membrane peroxidation and intracellular reactive oxygen species formation. In addition, the formation of multicellular microspheres before encapsulation maximized cell–cell contacts and increased viability of SMG cells over 14-day culture periods. Thiol-ene hydrogel-encapsulated microspheres also promoted SMG proliferation. Lineage tracing was employed to determine the cellular composition of hydrogel-encapsulated microspheres using markers for acinar (Mist1) and duct (Keratin5) cells. Our findings indicate that both acinar and duct cell phenotypes are present throughout the 14 day culture period. However, the acinar:duct cell ratios are reduced over time, likely due to duct cell proliferation. Altogether, permissive encapsulation methods for primary SMG cells have been identified that promote cell viability, proliferation, and maintenance of differentiated salivary gland cell phenotypes, which allows for translation of this approach for salivary gland tissue engineering applications. PMID:25762214

Tailoring the degradation rates of thermally responsive hydrogels designed for soft tissue injection by varying the autocatalytic potential.

PubMed

Zhu, Yang; Jiang, Hongbin; Ye, Sang-Ho; Yoshizumi, Tomo; Wagner, William R

2015-01-01

The ability to modulate the degradation properties of biomaterials such as thermally responsive hydrogels is desirable when exploring new therapeutic strategies that rely on the temporary presence of a placed scaffold or gel. Here we report a method of manipulating the absorption rate of a poly(N-isopropylacrylamide) ((poly(NIPAAm)) based hydrogel across a wide range (from 1 d to 5 mo) by small alterations in the composition. Relying upon the autocatalytic effect, the degradation of poly(NIPAAm-co-HEMA-co-MAPLA), (HEMA = 2-hydroxyethyl methacrylate; MAPLA = methacrylate-polylactide) was greatly accelerated by adding a fourth monomer methacrylic acid (MAA) at no more than 2 mol% to obtain poly(NIPAAm-co-HEMA-co-MAPLA-co-MAA) (pNHMMj) where j reflects the MAA molar % in the reactant mixture. MAA residue introduction decreased the pH inside the hydrogels and in surrounding buffered solutions. Accelerated degradation positively correlated with MAA content in pNHMMj polymers, putatively by the accelerated cleavage of MAPLA residues to raise the transition temperature of the polymer above body temperature. Physical properties including thermal transition behavior and initial mechanical strength did not vary significantly with MAA content. A rat hindlimb injection model generally reflected the in vitro observation that higher MAA content resulted in more rapid degradation and cellular infiltration. The strategy of tuning the degradation of thermally responsive hydrogels where degradation or solubilization is determined by their polyester components might be applied to other tissue engineering and regenerative medicine applications where designed biomaterial degradation behavior is needed. Copyright © 2015 Elsevier Ltd. All rights reserved.

Biofunctionalized peptide-based hydrogels provide permissive scaffolds to attract neurite outgrowth from spiral ganglion neurons.

PubMed

Frick, Claudia; Müller, Marcus; Wank, Ute; Tropitzsch, Anke; Kramer, Benedikt; Senn, Pascal; Rask-Andersen, Helge; Wiesmüller, Karl-Heinz; Löwenheim, Hubert

2017-01-01

Cochlear implants (CI) allow for hearing rehabilitation in patients with sensorineural hearing loss or deafness. Restricted CI performance results from the spatial gap between spiral ganglion neurons and the CI, causing current spread that limits spatially restricted stimulation and impairs frequency resolution. This may be substantially improved by guiding peripheral processes of spiral ganglion neurons towards and onto the CI electrode contacts. An injectable, peptide-based hydrogel was developed which may provide a permissive scaffold to facilitate neurite growth towards the CI. To test hydrogel capacity to attract spiral ganglion neurites, neurite outgrowth was quantified in an in vitro model using a custom-designed hydrogel scaffold and PuraMatrix ® . Neurite attachment to native hydrogels is poor, but significantly improved by incorporation of brain-derived neurotrophic factor (BDNF), covalent coupling of the bioactive laminin epitope IKVAV and the incorporation a full length laminin to hydrogel scaffolds. Incorporation of full length laminin protein into a novel custom-designed biofunctionalized hydrogel (IKVAV-GGG-SIINFEKL) allows for neurite outgrowth into the hydrogel scaffold. The study demonstrates that peptide-based hydrogels can be specifically biofunctionalized to provide a permissive scaffold to attract neurite outgrowth from spiral ganglion neurons. Such biomaterials appear suitable to bridge the spatial gap between neurons and the CI. Copyright © 2016 Elsevier B.V. All rights reserved.

Advances in Carbon Nanotubes-Hydrogel Hybrids in Nanomedicine for Therapeutics.

PubMed

Vashist, Arti; Kaushik, Ajeet; Vashist, Atul; Sagar, Vidya; Ghosal, Anujit; Gupta, Y K; Ahmad, Sharif; Nair, Madhavan

2018-05-01

In spite of significant advancement in hydrogel technology, low mechanical strength and lack of electrical conductivity have limited their next-level biomedical applications for skeletal muscles, cardiac and neural cells. Host-guest chemistry based hybrid nanocomposites systems have gained attention as they completely overcome these pitfalls and generate bioscaffolds with tunable electrical and mechanical characteristics. In recent years, carbon nanotube (CNT)-based hybrid hydrogels have emerged as innovative candidates with diverse applications in regenerative medicines, tissue engineering, drug delivery devices, implantable devices, biosensing, and biorobotics. This article is an attempt to recapitulate the advancement in synthesis and characterization of hybrid hydrogels and provide deep insights toward their functioning and success as biomedical devices. The improved comparative performance and biocompatibility of CNT-hydrogels hybrids systems developed for targeted biomedical applications are addressed here. Recent updates toward diverse applications and limitations of CNT hybrid hydrogels is the strength of the review. This will provide a holistic approach toward understanding of CNT-based hydrogels and their applications in nanotheranostics. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Transient Dynamic Mechanical Analysis of Resilin-based Elastomeric Hydrogels

NASA Astrophysics Data System (ADS)

Li, Linqing; Kiick, Kristi

2014-04-01

The outstanding high-frequency properties of emerging resilin-like polypeptides (RLPs) have motivated their development for vocal fold tissue regeneration and other applications. Recombinant RLP hydrogels show efficient gelation, tunable mechanical properties, and display excellent extensibility, but little has been reported about their transient mechanical properties. In this manuscript, we describe the transient mechanical behavior of new RLP hydrogels investigated via both sinusoidal oscillatory shear deformation and uniaxial tensile testing. Oscillatory stress relaxation and creep experiments confirm that RLP-based hydrogels display significantly reduced stress relaxation and improved strain recovery compared to PEG-based control hydrogels. Uniaxial tensile testing confirms the negligible hysteresis, reversible elasticity and superior resilience (up to 98%) of hydrated RLP hydrogels, with Young’s modulus values that compare favorably with those previously reported for resilin and that mimic the tensile properties of the vocal fold ligament at low strain (< 15%). These studies expand our understanding of the properties of these RLP materials under a variety of conditions, and confirm the unique applicability, for mechanically demanding tissue engineering applications, of a range of RLP hydrogels.

Programmable Hydrogels for Cell Encapsulation and Neo-Tissue Growth to Enable Personalized Tissue Engineering.

PubMed

Bryant, Stephanie J; Vernerey, Franck J

2018-01-01

Biomimetic and biodegradable synthetic hydrogels are emerging as a promising platform for cell encapsulation and tissue engineering. Notably, synthetic-based hydrogels offer highly programmable macroscopic properties (e.g., mechanical, swelling and transport properties) and degradation profiles through control over several tunable parameters (e.g., the initial network structure, degradation kinetics and behavior, and polymer properties). One component to success is the ability to maintain structural integrity as the hydrogel transitions to neo-tissue. This seamless transition is complicated by the fact that cellular activity is highly variable among donors. Thus, computational models provide an important tool in tissue engineering due to their unique ability to explore the coupled processes of hydrogel degradation and neo-tissue growth across multiple length scales. In addition, such models provide new opportunities to develop predictive computational tools to overcome the challenges with designing hydrogels for different donors. In this report, programmable properties of synthetic-based hydrogels and their relation to the hydrogel's structural properties and their evolution with degradation are reviewed. This is followed by recent progress on the development of computational models that describe hydrogel degradation with neo-tissue growth when cells are encapsulated in a hydrogel. Finally, the potential for predictive models to enable patient-specific hydrogel designs for personalized tissue engineering is discussed. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Visible light induced electropolymerization of suspended hydrogel bioscaffolds in a microfluidic chip.

PubMed

Li, Pan; Yu, Haibo; Liu, Na; Wang, Feifei; Lee, Gwo-Bin; Wang, Yuechao; Liu, Lianqing; Li, Wen Jung

2018-05-23

The development of microengineered hydrogels co-cultured with cells in vitro could advance in vivo bio-systems in both structural complexity and functional hierarchy, which holds great promise for applications in regenerative tissues or organs, drug discovery and screening, and bio-sensors or bio-actuators. Traditional hydrogel microfabrication technologies such as ultraviolet (UV) laser or multiphoton laser stereolithography and three-dimensional (3D) printing systems have advanced the development of 3D hydrogel micro-structures but need either expensive and complex equipment, or harsh material selection with limited photoinitiators. Herein, we propose a simple and flexible hydrogel microfabrication method based on a ubiquitous visible-light projection system combined with a custom-designed photosensitive microfluidic chip, to rapidly (typically several to tens of seconds) fabricate various two-dimensional (2D) hydrogel patterns and 3D hydrogel constructs. A theoretical layer-by-layer model that involves continuous polymerizing-delaminating-polymerizing cycles is presented to explain the polymerization and structural formation mechanism of hydrogels. A large area of hydrogel patterns was efficiently fabricated without the usage of costly laser systems or photoinitiators, i.e., a stereoscopic mesh-like hydrogel network with intersecting hydrogel micro-belts was fabricated via a series of dynamic-changing digital light projections. The pores and gaps of the hydrogel network are tunable, which facilitates the supply of nutrients and discharge of waste in the construction of 3D thick bio-models. Cell co-culture experiments showed the effective regulation of cell spreading by hydrogel scaffolds fabricated by the new method presented here. This visible light enabled hydrogel microfabrication method may provide new prospects for designing cell-based units for advanced biomedical studies, e.g., for 3D bio-models or bio-actuators in the future.

Bacterial cellulose based hydrogel (BC-g-AA) and preliminary result of swelling behavior

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hakam, Adil; Lazim, Azwan Mat; Abdul Rahman, I. Irman

2013-11-27

In this study, hydrogel based on Bacterial cellulose (BC) or local known as Nata de Coco, which grafted with monomer: Acrylic acid (AA) is synthesis by using gamma radiation technique. These hydrogel (BC-g-AA) has unique characteristic whereby responsive to pH buffer solution.

Synthesis and evaluation on pH- and temperature-responsive chitosan-p(MAA-co-NIPAM) hydrogels.

PubMed

Rasib, S Z M; Ahmad, Z; Khan, A; Akil, H M; Othman, M B H; Hamid, Z A A; Ullah, F

2018-03-01

In this study, chitosan-poly(methacrylic acid-co-N-isopropylacrylamide) [chitosan-p(MAA-co-NIPAM)] hydrogels were synthesized by emulsion polymerization. In order to be used as a carrier for drug delivery systems, the hydrogels had to be biocompatible, biodegradable and multi-responsive. The polymerization was performed by copolymerize MAA and NIPAM with chitosan polymer to produce a chitosan-based hydrogel. Due to instability during synthesis and complexity of components to produce the hydrogel, further study at different times of reaction is important to observe the synthesis process, the effect of end product on swelling behaviour and the most important is to find the best way to control the hydrogel synthesis in order to have an optimal swelling behaviour for drug release application. Studied by using Fourier transform infra-red (FTIR) spectroscopy found that, the synthesized was successfully produced stable chitosan-based hydrogel with PNIPAM continuously covered the outer surface of hydrogel which influenced much on the stability during synthesis. The chitosan and PMAA increased the zeta potential of the hydrogel and the chitosan capable to control shrinkage above human body temperature. The chitosan-p(MAA-co-NIPAM) hydrogels also responses to pH and temperature thus improved the ability to performance as a drug carrier. Copyright © 2017 Elsevier B.V. All rights reserved.

Influence of Different ECM-Like Hydrogels on Neurite Outgrowth Induced by Adipose Tissue-Derived Stem Cells

PubMed Central

Oliveira, E.; Assunção-Silva, R. C.; Teixeira, F. G.

2017-01-01

Mesenchymal stem cells (MSCs) have been proposed for spinal cord injury (SCI) applications due to their capacity to secrete growth factors and vesicles—secretome—that impacts important phenomena in SCI regeneration. To improve MSC survival into SCI sites, hydrogels have been used as transplantation vehicles. Herein, we hypothesized if different hydrogels could interact differently with adipose tissue-derived MSCs (ASCs). The efficacy of three natural hydrogels, gellan gum (functionalized with a fibronectin peptide), collagen, and a hydrogel rich in laminin epitopes (NVR-gel) in promoting neuritogenesis (alone and cocultured with ASCs), was evaluated in the present study. Their impact on ASC survival, metabolic activity, and gene expression was also evaluated. Our results indicated that all hydrogels supported ASC survival and viability, being this more evident for the functionalized GG hydrogels. Moreover, the presence of different ECM-derived biological cues within the hydrogels appears to differently affect the mRNA levels of growth factors involved in neuronal survival, differentiation, and axonal outgrowth. All the hydrogel-based systems supported axonal growth mediated by ASCs, but this effect was more robust in functionalized GG. The data herein presented highlights the importance of biological cues within hydrogel-based biomaterials as possible modulators of ASC secretome and its effects for SCI applications. PMID:29333166

A glucose-sensitive block glycopolymer hydrogel based on dynamic boronic ester bonds for insulin delivery.

PubMed

Cai, Baoqi; Luo, Yanping; Guo, Qianqian; Zhang, Xinge; Wu, Zhongming

2017-06-05

Hydrogels are good candidates to satisfy many needs for functional and tunable biomaterials. How to precisely control the gel structure and functions is crucial for the construction of sophisticated soft biomaterials comprising the hydrogels, which facilitates the impact of the surrounding environment on a unique biological function occurring. Here, glucose-responsive hydrogels comprised of 3-acrylamidophenyl boronic acid copolymerized with 2-lactobionamidoethyl methacrylate (p(APBA-b-LAMA)) were synthesized, and further evaluated as carriers for insulin delivery. The formation of (p(APBA-b-LAMA)) hydrogel was based on dynamic covalent bond using the association of boronic acid with diols. P(APBA-b-LAMA) hydrogel with the typical porous structure showed a rapid increase in equilibrium of swelling, which was up to 1856% after incubation with aqueous solution. Using insulin as a model protein therapeutic, p(APBA-b-LAMA) hydrogel exhibited high drug loading capability up to 15.6%, and also displayed glucose-dependent insulin release under physiological conditions. Additionally, the viability of NIH3T3 cells was more than 90% after treated with p(APBA-b-LAMA) hydrogel, indicating that the hydrogel had no cytotoxicity. Consequently, the novel p(APBA-b-LAMA) hydrogel has a practical application for diabetes treatment. Copyright © 2017. Published by Elsevier Ltd.

Biodegradable HEMA-based hydrogels with enhanced mechanical properties.

PubMed

Moghadam, Mohamadreza Nassajian; Pioletti, Dominique P

2016-08-01

Hydrogels are widely used in the biomedical field. Their main purposes are either to deliver biological active agents or to temporarily fill a defect until they degrade and are followed by new host tissue formation. However, for this latter application, biodegradable hydrogels are usually not capable to sustain any significant load. The development of biodegradable hydrogels presenting load-bearing capabilities would open new possibilities to utilize this class of material in the biomedical field. In this work, an original formulation of biodegradable photo-crosslinked hydrogels based on hydroxyethyl methacrylate (HEMA) is presented. The hydrogels consist of short-length poly(2-hydroxyethyl methacrylate) (PHEMA) chains in a star shape structure, obtained by introducing a tetra-functional chain transfer agent in the backbone of the hydrogels. They are cross-linked with a biodegradable N,O-dimethacryloyl hydroxylamine (DMHA) molecule sensitive to hydrolytic cleavage. We characterized the degradation properties of these hydrogels submitted to mechanical loadings. We showed that the developed hydrogels undergo long-term degradation and specially meet the two essential requirements of a biodegradable hydrogel suitable for load bearing applications: enhanced mechanical properties and low molecular weight degradation products. © 2015 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 104B: 1161-1169, 2016. © 2015 Wiley Periodicals, Inc.

Cellularizing hydrogel-based scaffolds to repair bone tissue: How to create a physiologically relevant micro-environment?

PubMed Central

Maisani, Mathieu; Pezzoli, Daniele; Chassande, Olivier; Mantovani, Diego

2017-01-01

Tissue engineering is a promising alternative to autografts or allografts for the regeneration of large bone defects. Cell-free biomaterials with different degrees of sophistication can be used for several therapeutic indications, to stimulate bone repair by the host tissue. However, when osteoprogenitors are not available in the damaged tissue, exogenous cells with an osteoblast differentiation potential must be provided. These cells should have the capacity to colonize the defect and to participate in the building of new bone tissue. To achieve this goal, cells must survive, remain in the defect site, eventually proliferate, and differentiate into mature osteoblasts. A critical issue for these engrafted cells is to be fed by oxygen and nutrients: the transient absence of a vascular network upon implantation is a major challenge for cells to survive in the site of implantation, and different strategies can be followed to promote cell survival under poor oxygen and nutrient supply and to promote rapid vascularization of the defect area. These strategies involve the use of scaffolds designed to create the appropriate micro-environment for cells to survive, proliferate, and differentiate in vitro and in vivo. Hydrogels are an eclectic class of materials that can be easily cellularized and provide effective, minimally invasive approaches to fill bone defects and favor bone tissue regeneration. Furthermore, by playing on their composition and processing, it is possible to obtain biocompatible systems with adequate chemical, biological, and mechanical properties. However, only a good combination of scaffold and cells, possibly with the aid of incorporated growth factors, can lead to successful results in bone regeneration. This review presents the strategies used to design cellularized hydrogel-based systems for bone regeneration, identifying the key parameters of the many different micro-environments created within hydrogels. PMID:28634532

Using In situ Dynamic Cultures to Rapidly Biofabricate Fabric-Reinforced Composites of Chitosan/Bacterial Nanocellulose for Antibacterial Wound Dressings

PubMed Central

Zhang, Peng; Chen, Lin; Zhang, Qingsong; Hong, Feng F.

2016-01-01

Bacterial nano-cellulose (BNC) is considered to possess incredible potential in biomedical applications due to its innate unrivaled nano-fibrillar structure and versatile properties. However, its use is largely restricted by inefficient production and by insufficient strength when it is in a highly swollen state. In this study, a fabric skeleton reinforced chitosan (CS)/BNC hydrogel with high mechanical reliability and antibacterial activity was fabricated by using an efficient dynamic culture that could reserve the nano-fibrillar structure. By adding CS in culture media to 0.25–0.75% (w/v) during bacterial cultivation, the CS/BNC composite hydrogel was biosynthesized in situ on a rotating drum composed of fabrics. With the proposed method, BNC biosynthesis became less sensitive to the adverse antibacterial effects of CS and the production time of the composite hydrogel with desirable thickness could be halved from 10 to 5 days as compared to the conventional static cultures. Although, its concentration was low in the medium, CS accounted for more than 38% of the CS/BNC dry weight. FE-SEM observation confirmed conservation of the nano-fibrillar networks and covering of CS on BNC. ATR-FTIR showed a decrease in the degree of intra-molecular hydrogen bonding and water absorption capacity was improved after compositing with CS. The fabric-reinforced CS/BNC composite exhibited bacteriostatic properties against Escherichia coli and Staphylococcus aureus and significantly improved mechanical properties as compared to the BNC sheets from static culture. In summary, the fabric-reinforced CS/BNC composite constitutes a desired candidate for advanced wound dressings. From another perspective, coating of BNC or CS/BNC could upgrade the conventional wound dressings made of cotton gauze to reduce pain during wound healing, especially for burn patients. PMID:26973634

Interfacial self-healing of nanocomposite hydrogels: Theory and experiment

NASA Astrophysics Data System (ADS)

Wang, Qiming; Gao, Zheming; Yu, Kunhao

2017-12-01

Polymers with dynamic bonds are able to self-heal their fractured interfaces and restore the mechanical strengths. It is largely elusive how to analytically model this self-healing behavior to construct the mechanistic relationship between the self-healing properties (e.g., healed interfacial strength and equilibrium healing time) and the material compositions and healing conditions. Here, we take a self-healable nanocomposite hydrogel as an example to illustrate an interfacial self-healing theory for hydrogels with dynamic bonds. In the theory, we consider the free polymer chains diffuse across the interface and reform crosslinks to bridge the interface. We analytically reveal that the healed strengths of nanocomposite hydrogels increase with the healing time in an error-function-like form. The equilibrium self-healing time of the full-strength recovery decreases with the temperature and increases with the nanoparticle concentration. We further analytically reveal that the healed interfacial strength decreases with increasing delaying time before the healing process. The theoretical results quantitatively match with our experiments on nanosilica hydrogels, and also agree well with other researchers' experiments on nanoclay hydrogels. We expect that this theory would open promising avenues for quantitative understanding of the self-healing mechanics of various polymers with dynamic bonds, and offer insights for designing high-performance self-healing polymers.

Optimization of gatifloxacin liposomal hydrogel for enhanced transcorneal permeation.

PubMed

Hosny, Khaled Mohamed

2010-03-01

The aim of this study was to prepare and characterize a topically effective prolonged-release ophthalmic gatifloxacin liposomal hydrogel formulation. Reverse-phase evaporation was used for the preparation of liposomes consisting of phosphatidylcholine (PC) and cholesterol (CH). The effect of PC:CH molar ratio on the percentage of drug encapsulated was investigated. The effect of additives, such as stearylamine (SA) or dicetyl phosphate (DP), as positive and negative charge inducers, respectively, was studied. Morphology, mean size, encapsulation efficiency, and in vitro release of gatifloxacin from liposomes were evaluated. For hydrogel preparation, carbopol 940 was applied. In vitro transcorneal permeation through excised albino rabbit cornea was also determined. Optimal encapsulation efficiency was found at the 5:3 PC:CH molar ratio; by increasing CH content above this limit, the encapsulation efficiency decreased. Positively charged liposomes showed superior entrapment efficiency over other liposomes. Hydrogel-containing liposomes with lipid content PC, CH, and SA in a molar ratio of 5:3:1, respectively, showed best release and transcorneal permeation. These results suggest that the encapsulation of gatifloxacin into liposomes prolonged the in vitro release, depending on composition of the vesicles. In addition, the polymer hydrogel used in the preparation ensured steady, prolonged transcorneal permeation. In conclusion, gatifloxacin liposomal hydrogel is a suitable delivery system for the improvement of the ocular bioavailability of gatifloxacin.

In vivo evaluation of the bone integration of coated poly(vinyl-alcohol) hydrogel fiber implants.

PubMed

Moreau, David; Villain, Arthur; Bachy, Manon; Proudhon, Henry; Ku, David N; Hannouche, Didier; Petite, Hervé; Corté, Laurent

2017-08-01

Recently, it has been shown that constructs of poly(vinyl alcohol) (PVA) hydrogel fibers reproduce closely the tensile behavior of ligaments. However, the biological response to these systems has not been explored yet. Here, we report the first in vivo evaluation of these implants and focus on the integration in bone, using a rabbit model of bone tunnel healing. Implants consisted in bundles of PVA hydrogel fibers embedded in a PVA hydrogel matrix. Half of the samples were coated with a composite coating of hydroxyapatite (HA) particles embedded in PVA hydrogel. The biological integration was evaluated at 6 weeks using histology and micro-CT imaging. For all implants, a good biological tolerance and growth of new bone tissue are reported. All the implants were surrounded by a fibrous layer comparable to what was previously observed for poly(ethylene terephthalate) (PET) fibers currently used in humans for ligament reconstruction. An image analysis method is proposed to quantify the thickness of this fibrous capsule. Implants coated with HA were not significantly osteoconductive, which can be attributed to the slow dissolution of the selected hydroxyapatite. Overall, these results confirm the relevance of PVA hydrogel fibers for ligament reconstruction and adjustments are proposed to enhance its osseointegration.

Design and synthesis of an amphiphilic graft hydrogel having a hydrophobic domain formed by multiple interactions.

PubMed

Nitta, Kyohei; Kimoto, Atsushi; Watanabe, Junji

2016-11-01

A novel hydrogel having hydrophobic oligo segments and hydrophilic poly(acrylamidoglycolic acid) (PAGA) as pH responsive polymer segments was designed and synthesized to be used as a soft biomaterial. Poly(trimethylene carbonate) (PTMC) as the side chain, for which the degrees of polymerization were 9, 19, and 49, and the composition ratios were 1, 5, and 10mol%, was used as the oligo segment in the hydrogel. The swelling ratio of the hydrogel was investigated under various changes in conditions such as pH, temperature, and hydrogen bonding upon urea addition. Under pH2-11 conditions, the graft gel reversibly swelled and shrank due to the effect of PAGA main chain. The interior morphology and skin layer of the hydrogel was observed by a scanning electron microscope. The hydrogel composed of PAGA as the hydrophilic polymer backbone had a sponge-like structure, with a pore size of approximately 100μm. On the other hand, upon increasing the ratio of trimethylene carbonate (TMC) units in the hydrogel, the pores became smaller or disappeared. Moreover, thickness of the skin layer significantly increased with the swelling ratio depended on the incorporation ratios of the PTMC macromonomer. Molecular incorporation in the hydrogel was evaluated using a dye as a model drug molecule. These features would play an important role in drug loading. Increasing the ratio of TMC units favored the adsorption of the dye and activation of the incorporation behavior. Copyright © 2016 Elsevier B.V. All rights reserved.

Advanced 3D Ni(OH)2/CNT Gel Composite Electrodes for Supercapacitors

NASA Astrophysics Data System (ADS)

Cheng, Hanlin; Duong, Hai Minh

2015-03-01

In order to enhance the performance of supercapacitors, advanced 3D Porous CNT/Ni(OH)2 gel composite electrodes are developed in this work. Compared with previously reported graphene gel supercapacitors, our electrodes using 1D CNTs have smaller diffusion resistance due to a shorter ion transport path. The developed 3D xerogel composite electrodes demonstrate the success of a careful engineered guest/host materials interface. Initially, the CNT gels are coated on the nickel foam to form a 3D scaffold, which serves as a microscopic electrical conductive network. Then Ni(OH)2 are incorporated using a traditional electrodeposition method. In this work, two types of the 3D CNT-coated nickel foams are investigated. The gels can be used directly as hydrogels or dried in air to form xerogels. Both hydrogels and xerogels present 3D tangled CNT networks. It shows that the hydrogel composite electrodes with unbundled CNTs, though presenting high capacitances of 1400 F/g at low discharge rate, possess lower capacitances at higher discharge rate and a poor cycling performance of less than 23% retention. In contrast, the xerogel composite electrodes can overcome these limitations in terms of a satisfied discharge performance of 1200 F/g and a good cycling retention more than 85% due to a stronger Ni(OH)2/CNT interface. The CNT bundles in the xerogel electrodes formed during the drying process can give a flat surface with small curvature, which facilitate the Ni(OH)2 nucleation and growth. Thanks for the support from the A star R-265-000-424-305.

Bioinspired Smart Actuator Based on Graphene Oxide-Polymer Hybrid Hydrogels.

PubMed

Wang, Tao; Huang, Jiahe; Yang, Yiqing; Zhang, Enzhong; Sun, Weixiang; Tong, Zhen

2015-10-28

Rapid response and strong mechanical properties are desired for smart materials used in soft actuators. A bioinspired hybrid hydrogel actuator was designed and prepared by series combination of three trunks of tough polymer-clay hydrogels to accomplish the comprehensive actuation of "extension-grasp-retraction" like a fishing rod. The hydrogels with thermo-creep and thermo-shrinking features were successively irradiated by near-infrared (NIR) to execute extension and retraction, respectively. The GO in the hydrogels absorbed the NIR energy and transformed it into thermo-energy rapidly and effectively. The hydrogel with adhesion or magnetic force was adopted as the "hook" of the hybrid hydrogel actuator for grasping object. The hook of the hybrid hydrogel actuator was replaceable according to applications, even with functional materials other than hydrogels. This study provides an innovative concept to explore new soft actuators through combining response hydrogels and programming the same stimulus.

Poly(ethylene glycol) hydrogel microstructures encapsulating living cells

NASA Technical Reports Server (NTRS)

Koh, Won-Gun; Revzin, Alexander; Pishko, Michael V.

2002-01-01

We present an easy and effective method for the encapsulation of cells inside PEG-based hydrogel microstructures fabricated using photolithography. High-density arrays of three-dimensional microstructures were created on substrates using this method. Mammalian cells were encapsulated in cylindrical hydrogel microstructures of 600 and 50 micrometers in diameter or in cubic hydrogel structures in microfluidic channels. Reducing lateral dimension of the individual hydrogel microstructure to 50 micrometers allowed us to isolate 1-3 cells per microstructure. Viability assays demonstrated that cells remained viable inside these hydrogels after encapsulation for up to 7 days.

Programmable Matter Creating Systems that Can Think, Talk, and Morph Autonomously. Phase 2

DTIC Science & Technology

2011-09-13

irradiation. SWNTs have a well-defined near-IR optical absorption, specifically ideal for biocompatible devices such as drug delivery mediums or biological...investigated as follows: • Lower Critical Transition Temperature(LCST) of the CNT-pNIPAM composites. • Strain change of CNT-pNIPAM hydrogel at LCST...loading at concentrations of 0.75mg/mL, we demonstrate up to 5 times enhancement to the thermal response time of the nanotube- pNIPAM hydrogel

Preparation and characterisation of a novel hydrogel based on Auricularia polytricha β-glucan and its bio-release property for vitamin B12 delivery.

PubMed

Zhu, Kai; Chen, Xiaoyuan; Yu, Da; He, Yue; Song, Guanglei

2018-05-01

This study investigates a novel hydrogel synthesis method and its bio-release property. This hydrogel, with a three-dimensional network structure based on Auricularia polytricha β-glucan, was characterised by means of Fourier transform infrared spectroscopy, 1 H NMR and scanning electron microscopy. Vitamin B 12 (VB 12 , cobalamin) as a hydrophilic functional food component was entrapped into these hydrogels. The in vitro release profile of VB 12 was established in simulated gastric fluid (SGF) and simulated intestinal fluid (SIF). The results showed that the hydrogel had medium pore size from 30 to 300 µm, and the swelling ratio increased with the degree of substitution. The hydrogel demonstrated good stability in SGF and bio-release capability in SIF for VB 12 . The accumulated release rate is about 80% in SIF and below 20% in SGF, which indicated the significant different release property in stomach and intestine. The Auricularia polytricha β-glucan-based hydrogel has a good swelling ratio, pepsin stability and pancrelipase-catalysed biodegradation property. The bio-release rate is significantly different in SIF and SGF, which indicated that this hydrogel could be a good intestinal target carrier of VB 12 . © 2017 Society of Chemical Industry. © 2017 Society of Chemical Industry.

Controlled Assembly of Rod-Like Particles

DTIC Science & Technology

2012-11-29

Thompson, Shaojin You, Qian Wang. M13 bacteriophage-polymer nanoassemblies as drug delivery vehicles, Nano Research, (02 2011): 483. doi: 10.1007...virus-based composite nanofibers , Journal of Materials Chemistry, (06 2011): 0. doi: 10.1039/c1jm00078k 10/20/2011 8.00 Sumit Kewalramani, Suntao Wang...exploited to dictate the order that emerges in many-body assemblies. (2) Incorporation of TMV into alginate hydrogels As shown in Figure 1, we recently

Biomass-derived sponge-like carbonaceous hydrogels and aerogels for supercapacitors.

PubMed

Wu, Xi-Lin; Wen, Tao; Guo, Hong-Li; Yang, Shubin; Wang, Xiangke; Xu, An-Wu

2013-04-23

As a newly developed material, carbon gels have been receiving considerable attention due to their multifunctional properties. Herein, we present a facile, green, and template-free route toward sponge-like carbonaceous hydrogels and aerogels by using crude biomass, watermelon as the carbon source. The obtained three-dimensional (3D) flexible carbonaceous gels are made of both carbonaceous nanofibers and nanospheres. The porous carbonaceous gels (CGs) are highly chemically active and show excellent mechanical flexibility which enable them to be a good scaffold for the synthesis of 3D composite materials. We synthesized the carbonaceous gel-based composite materials by incorporating Fe3O4 nanoparticles into the networks of the carbonaceous gels. The Fe3O4/CGs composites further transform into magnetite carbon aerogels (MCAs) by calcination. The MCAs keep the porous structure of the original CGs, which allows the sustained and stable transport of both electrolyte ions and electrons to the electrode surface, leading to excellent electrochemical performance. The MCAs exhibit an excellent capacitance of 333.1 F·g(-1) at a current density of 1 A·g(-1) within a potential window of -1.0 to 0 V in 6 M KOH solution. Meanwhile, the MCAs also show outstanding cycling stability with 96% of the capacitance retention after 1000 cycles of charge/discharge. These findings open up the use of low-cost elastic carbon gels for the synthesis of other 3D composite materials and show the possibility for the application in energy storage.

Microfluidic hydrogels for tissue engineering.

PubMed

Huang, Guo You; Zhou, Li Hong; Zhang, Qian Cheng; Chen, Yong Mei; Sun, Wei; Xu, Feng; Lu, Tian Jian

2011-03-01

With advanced properties similar to the native extracellular matrix, hydrogels have found widespread applications in tissue engineering. Hydrogel-based cellular constructs have been successfully developed to engineer different tissues such as skin, cartilage and bladder. Whilst significant advances have been made, it is still challenging to fabricate large and complex functional tissues due mainly to the limited diffusion capability of hydrogels. The integration of microfluidic networks and hydrogels can greatly enhance mass transport in hydrogels and spatiotemporally control the chemical microenvironment of cells, mimicking the function of native microvessels. In this review, we present and discuss recent advances in the fabrication of microfluidic hydrogels from the viewpoint of tissue engineering. Further development of new hydrogels and microengineering technologies will have a great impact on tissue engineering.

Preparation and physico-chemical properties of hydrogels from carboxymethyl cassava starch crosslinked with citric acid

NASA Astrophysics Data System (ADS)

Boonkham, Sasikan; Sangseethong, Kunruedee; Chatakanon, Pathama; Niamnuy, Chalida; Nakasaki, Kiyohiko; Sriroth, Klanarong

2014-06-01

Recently, environmentally friendly hydrogels prepared from renewable bio-based resources have drawn significant attention from both industrial and academic sectors. In this study, chemically crosslinked hydrogels have been developed from cassava starch which is a bio-based polymer using a non-toxic citric acid as a crosslinking agent. Cassava starch was first modified by carboxymethylation to improve its water absorbency property. The carboxymethyl cassava starch (CMCS) obtained was then crosslinked with citric acid at different concentrations and reaction times. The gel fraction of hydrogels increased progressively with increasing citric acid concentration. Free swelling capacity of hydrogels in de-ionized water, saline solution and buffers at various pHs as well as absorption under load were investigated. The results revealed that swelling behavior and mechanical characteristic of hydrogels depended on the citric acid concentration used in reaction. Increasing citric acid concentration resulted in hydrogels with stronger network but lower swelling and absorption capacity. The cassava starch hydrogels developed were sensitive to ionic strength and pH of surrounding medium, showing much reduced swelling capacity in saline salt solution and acidic buffers.

UV-crosslinkable and thermo-responsive chitosan hybrid hydrogel for NIR-triggered localized on-demand drug delivery.

PubMed

Wang, Lei; Li, Baoqiang; Xu, Feng; Xu, Zheheng; Wei, Daqing; Feng, Yujie; Wang, Yaming; Jia, Dechang; Zhou, Yu

2017-10-15

Innovative drug delivery technologies based on smart hydrogels for localized on-demand drug delivery had aroused great interest. To acquire smart UV-crosslinkable chitosan hydrogel for NIR-triggered localized on-demanded drug release, a novel UV-crosslinkable and thermo-responsive chitosan was first designed and synthesized by grafting with poly N-isopropylacrylamide, acetylation of methacryloyl groups and embedding with photothermal carbon. The UV-crosslinkable unit (methacryloyl groups) endowed chitosan with gelation via UV irradiation. The thermo-responsive unit (poly N-isopropylacrylamide) endowed chitosan hydrogel with temperature-triggered volume shrinkage and reversible swelling/de-swelling behavior. The chitosan hybrid hydrogel embedded with photothermal carbon exhibited distinct NIR-triggered volume shrinkage (∼42% shrinkage) in response to temperature elevation as induced by NIR laser irradiation. As a demonstration, doxorubicin release rate was accelerated and approximately 40 times higher than that from non-irradiated hydrogels. The UV-crosslinkable and thermal-responsive hybrid hydrogel served as in situ forming hydrogel-based drug depot is developed for NIR-triggered localized on-demand release. Copyright © 2017 Elsevier Ltd. All rights reserved.

An improved correlation to predict molecular weight between crosslinks based on equilibrium degree of swelling of hydrogel networks.

PubMed

Jimenez-Vergara, Andrea C; Lewis, John; Hahn, Mariah S; Munoz-Pinto, Dany J

2018-04-01

Accurate characterization of hydrogel diffusional properties is of substantial importance for a range of biotechnological applications. The diffusional capacity of hydrogels has commonly been estimated using the average molecular weight between crosslinks (M c ), which is calculated based on the equilibrium degree of swelling. However, the existing correlation linking M c and equilibrium swelling fails to accurately reflect the diffusional properties of highly crosslinked hydrogel networks. Also, as demonstrated herein, the current model fails to accurately predict the diffusional properties of hydrogels when polymer concentration and molecular weight are varied simultaneously. To address these limitations, we evaluated the diffusional properties of 48 distinct hydrogel formulations using two different photoinitiator systems, employing molecular size exclusion as an alternative methodology to calculate average hydrogel mesh size. The resulting data were then utilized to develop a revised correlation between M c and hydrogel equilibrium swelling that substantially reduces the limitations associated with the current correlation. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 106B: 1339-1348, 2018. © 2017 Wiley Periodicals, Inc.

Unperturbed volume transition of thermosensitive poly-(N-isopropylacrylamide) microgel particles embedded in a hydrogel matrix.

PubMed

Musch, Judith; Schneider, Stefanie; Lindner, Peter; Richtering, Walter

2008-05-22

The thermoresponsive behavior of poly-(N-isopropylacrylamide) (PNiPAM) microgels embedded in a covalently cross-linked polyacrylamide hydrogel matrix was investigated using ultraviolet-visible (UV-vis) spectroscopy, small-angle neutron scattering (SANS), and confocal laser scanning microscopy. The hydrogel synthesis was performed at two different temperatures, below and above the volume phase transition temperature of PNiPAM, resulting in highly swollen or fully collapsed PNiPAM microgel particles during the incorporation step. UV-vis spectroscopy experiments verify that the incorporation of thermosensitive microgels leads to temperature-sensitive optical properties of the composite materials. SANS measurements at different temperatures show that the thermosensitive swelling behavior of the PNiPAM microgels is fully retained in the composite material. Volume and structure criteria of the embedded microgel particles are compared to those of the free microgels in acrylamide solution. To visualize the temperature responsive behavior of larger PNiPAM particles, confocal fluorescence microscopy images of PNiPAM beads, of 40-microm size, were taken at two different temperatures. The micrographs also demonstrate the retained temperature sensitivity of the embedded microgels.

Stimuli-Responsive DNA-Based Hydrogels: From Basic Principles to Applications.

PubMed

Kahn, Jason S; Hu, Yuwei; Willner, Itamar

2017-04-18

The base sequence of nucleic acids encodes structural and functional information into the DNA biopolymer. External stimuli such as metal ions, pH, light, or added nucleic acid fuel strands provide triggers to reversibly switch nucleic acid structures such as metal-ion-bridged duplexes, i-motifs, triplex nucleic acids, G-quadruplexes, or programmed double-stranded hybrids of oligonucleotides (DNA). The signal-triggered oligonucleotide structures have been broadly applied to develop switchable DNA nanostructures and DNA machines, and these stimuli-responsive assemblies provide functional scaffolds for the rapidly developing area of DNA nanotechnology. Stimuli-responsive hydrogels undergoing signal-triggered hydrogel-to-solution transitions or signal-controlled stiffness changes attract substantial interest as functional matrices for controlled drug delivery, materials exhibiting switchable mechanical properties, acting as valves or actuators, and "smart" materials for sensing and information processing. The integration of stimuli-responsive oligonucleotides with hydrogel-forming polymers provides versatile means to exploit the functional information encoded in the nucleic acid sequences to yield stimuli-responsive hydrogels exhibiting switchable physical, structural, and chemical properties. Stimuli-responsive DNA-based nucleic acid structures are integrated in acrylamide polymer chains and reversible, switchable hydrogel-to-solution transitions of the systems are demonstrated by applying external triggers, such as metal ions, pH-responsive strands, G-quadruplex, and appropriate counter triggers that bridge and dissociate the polymer chains. By combining stimuli-responsive nucleic acid bridges with thermosensitive poly(N-isopropylacrylamide) (pNIPAM) chains, systems undergoing reversible solution ↔ hydrogel ↔ solid transitions are demonstrated. Specifically, by bridging acrylamide polymer chains by two nucleic acid functionalities, where one type of bridging unit provides a stimuli-responsive element and the second unit acts as internal "bridging memory", shape-memory hydrogels undergoing reversible and switchable transitions between shaped hydrogels and shapeless quasi-liquid states are demonstrated. By using stimuli-responsive hydrogel cross-linking units that can assemble the bridging units by two different input signals, the orthogonally-triggered functions of the shape-memory were shown. Furthermore, a versatile approach to assemble stimuli-responsive DNA-based acrylamide hydrogel films on surfaces is presented. The method involves the activation of the hybridization chain-reaction (HCR) by a surface-confined promoter strand, in the presence of acrylamide chains modified with two DNA hairpin structures and appropriate stimuli-responsive tethers. The resulting hydrogel-modified surfaces revealed switchable stiffness properties and signal-triggered catalytic functions. By applying the method to assemble the hydrogel microparticles, substrate-loaded, stimuli-responsive microcapsules are prepared. The signal-triggered DNA-based hydrogel microcapsules are applied as drug carriers for controlled release. The different potential applications and future perspectives of stimuli responsive hydrogels are discussed. Specifically, the use of these smart materials and assemblies as carriers for controlled drug release and as shape-memory matrices for information storage and inscription and the use of surface-confined stimuli-responsive hydrogels, exhibiting switchable stiffness properties, for catalysis and controlled growth of cells are discussed.

Functionalized graphene hydrogel-based high-performance supercapacitors.

PubMed

Xu, Yuxi; Lin, Zhaoyang; Huang, Xiaoqing; Wang, Yang; Huang, Yu; Duan, Xiangfeng

2013-10-25

Functionalized graphene hydrogels are prepared by a one-step low-temperature reduction process and exhibit ultrahigh specific capacitances and excellent cycling stability in the aqueous electrolyte. Flexible solid-state supercapacitors based on functionalized graphene hydrogels are demonstrated with superior capacitive performances and extraordinary mechanical flexibility. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Composite vascular scaffold combining electrospun fibers and physically-crosslinked hydrogel with copper wire-induced grooves structure.

PubMed

Liu, Yuanyuan; Jiang, Chen; Li, Shuai; Hu, Qingxi

2016-08-01

While the field of tissue engineered vascular grafts has greatly advanced, many inadequacies still exist. Successfully developed scaffolds require mechanical and structural properties that match native vessels and optimal microenvironments that foster cell integration, adhesion and growth. We have developed a small diameter, three-layered composite vascular scaffold which consists of electrospun fibers and physically-crosslinked hydrogel with copper wire-induced grooves by combining the electrospinning and dip-coating methods. Scaffold morphology and mechanics were assessed, quantified and compared to native vessels. Scaffolds were seeded with Human Umbilical Vein Endothelial Cells (HUVECs), cultured in vitro for 3 days and were evaluated for cell viability and morphology. The results showed that composite scaffolds had adjustable mechanical strength and favorable biocompatibility, which is important in the future clinical application of Tissue-engineered vascular grafts (TEVGs). Copyright © 2016 Elsevier Ltd. All rights reserved.

Lower irritation microemulsion-based rotigotine gel: formulation optimization and in vitro and in vivo studies.

PubMed

Wang, Zheng; Mu, Hong-Jie; Zhang, Xue-Mei; Ma, Peng-Kai; Lian, Sheng-Nan; Zhang, Feng-Pu; Chu, Sheng-Ying; Zhang, Wen-Wen; Wang, Ai-Ping; Wang, Wen-Yan; Sun, Kao-Xiang

2015-01-01

Rotigotine is a potent and selective D1, D2, and D3 dopaminergic receptor agonist. Due to an extensive first-pass effect, it has a very low oral bioavailability (approximately 0.5% in rats). The present investigation aimed to develop a microemulsion-based hydrogel for transdermal rotigotine delivery with lower application site reactions. Pseudoternary phase diagrams were constructed to determine the region of oil in water (o/w)-type microemulsion. Central composite design was used to support the pseudoternary phase diagrams and to select homogeneous and stable microemulsions with an optimal amount of rotigotine permeation within 24 hours. In vitro skin permeation experiments were performed, using Franz diffusion cells, to compare rotigotine-loaded microemulsions with rotigotine solutions in oil. The optimized formulation was used to prepare a microemulsion-based hydrogel, which was subjected to bioavailability and skin irritancy studies. The selected formulations of rotigotine-loaded microemulsions had enhanced flux and permeation coefficients compared with rotigotine in oil. The optimum microemulsion contained 68% water, 6.8% Labrafil(®), 13.44% Cremophor(®) RH40, 6.72% Labrasol(®), and 5.04% Transcutol(®) HP; the drug-loading rate was 2%. To form a microemulsion gel, 1% Carbomer 1342 was added to the microemulsion. The bioavailability of the rotigotine-loaded microemulsion gel was 105.76%±20.52% with respect to the marketed rotigotine patch (Neupro(®)). The microemulsion gel irritated the skin less than Neupro. A rotigotine microemulsion-based hydrogel was successfully developed, and an optimal formulation for drug delivery was identified. This product could improve patient compliance and have broad marketability.

A Triblock Copolymer Design Leads to Robust Hybrid Hydrogels for High-Performance Flexible Supercapacitors.

PubMed

Zhang, Guangzhao; Chen, Yunhua; Deng, Yonghong; Wang, Chaoyang

2017-10-18

We report here an intriguing hybrid conductive hydrogel as electrode for high-performance flexible supercapacitor. The key is using a rationally designed water-soluble ABA triblock copolymer (termed as IAOAI) containing a central poly(ethylene oxide) block (A) and terminal poly(acrylamide) (PAAm) block with aniline moieties randomly incorporated (B), which was synthesized by reversible additional fragment transfer polymerization. The subsequent copolymerization of aniline monomers with the terminated aniline moieties on the IAOAI polymer generates a three-dimensional cross-linking hybrid network. The hybrid hydrogel electrode demonstrates robust mechanical flexibility, remarkable electrochemical capacitance (919 F/g), and cyclic stability (90% capacitance retention after 1000 cycles). Moreover, the flexible supercapacitor based on this hybrid hydrogel electrode presents a large specific capacitance (187 F/g), superior to most reported conductive hydrogel-based supercapacitors. With the demonstrated additional favorable cyclic stability and excellent capacitive and rate performance, this hybrid hydrogel-based supercapacitor holds great promise for flexible energy-storage device.

Diffusion of water-soluble sorptive drugs in HEMA/MAA hydrogels.

PubMed

Liu, D E; Dursch, T J; Taylor, N O; Chan, S Y; Bregante, D T; Radke, C J

2016-10-10

We measure and, for the first time, theoretically predict four prototypical aqueous-drug diffusion coefficients in five soft-contact-lens material hydrogels where solute-specific adsorption is pronounced. Two-photon fluorescence confocal microscopy and UV/Vis-absorption spectrophotometry assess transient solute concentration profiles and concentration histories, respectively. Diffusion coefficients are obtained for acetazolamide, riboflavin, sodium fluorescein, and theophylline in 2-hydroxyethyl methacrylate/methacrylic acid (HEMA/MAA) copolymer hydrogels as functions of composition, equilibrium water content (30-90%), and aqueous pH (2 and 7.4). At pH2, MAA chains are nonionic, whereas at pH7.4, MAA chains are anionic (pKa≈5.2). All studied prototypical drugs specifically interact with HEMA and nonionic MAA (at pH2) moieties. Conversely, none of the prototypical drugs adsorb specifically to anionic MAA (at pH7.4) chains. As expected, diffusivities of adsorbing solutes are significantly diminished by specific interactions with hydrogel strands. Despite similar solute size, relative diffusion coefficients in the hydrogels span several orders of magnitude because of varying degrees of solute interactions with hydrogel-polymer chains. To provide a theoretical framework for the new diffusion data, we apply an effective-medium model extended for solute-specific interactions with hydrogel copolymer strands. Sorptive-diffusion kinetics is successfully described by local equilibrium and Henry's law. All necessary parameters are determined independently. Predicted diffusivities are in good agreement with experiment. Copyright © 2016 Elsevier B.V. All rights reserved.

Recent advances in clay mineral-containing nanocomposite hydrogels.

PubMed

Zhao, Li Zhi; Zhou, Chun Hui; Wang, Jing; Tong, Dong Shen; Yu, Wei Hua; Wang, Hao

2015-12-28

Clay mineral-containing nanocomposite hydrogels have been proven to have exceptional composition, properties, and applications, and consequently have attracted a significant amount of research effort over the past few years. The objective of this paper is to summarize and evaluate scientific advances in clay mineral-containing nanocomposite hydrogels in terms of their specific preparation, formation mechanisms, properties, and applications, and to identify the prevailing challenges and future directions in the field. The state-of-the-art of existing technologies and insights into the exfoliation of layered clay minerals, in particular montmorillonite and LAPONITE®, are discussed first. The formation and structural characteristics of polymer/clay nanocomposite hydrogels made from in situ free radical polymerization, supramolecular assembly, and freezing-thawing cycles are then examined. Studies indicate that additional hydrogen bonding, electrostatic interactions, coordination bonds, hydrophobic interaction, and even covalent bonds could occur between the clay mineral nanoplatelets and polymer chains, thereby leading to the formation of unique three-dimensional networks. Accordingly, the hydrogels exhibit exceptional optical and mechanical properties, swelling-deswelling behavior, and stimuli-responsiveness, reflecting the remarkable effects of clay minerals. With the pivotal roles of clay minerals in clay mineral-containing nanocomposite hydrogels, the nanocomposite hydrogels possess great potential as superabsorbents, drug vehicles, tissue scaffolds, wound dressing, and biosensors. Future studies should lay emphasis on the formation mechanisms with in-depth insights into interfacial interactions, the tactical functionalization of clay minerals and polymers for desired properties, and expanding of their applications.

Transport and Stability of Biological Molecules in Surfactant-Alginate Composite Hydrogels

PubMed Central

Stoppel, Whitney L.; White, Joseph C.; Horava, Sarena D.; Bhatia, Surita R.; Roberts, Susan C.

2013-01-01

Obstructed transport of biological molecules can result in improper release of pharmaceuticals or biologics from biomedical devices. Recent studies have shown that nonionic surfactants, such as Pluronic® F68 (F68), positively alter biomaterial properties, such as mesh size and microcapsule diameter. To further understand the effect of F68 (incorporated at concentrations well above the critical micelle concentration (CMC)) in traditional biomaterials, the transport properties of BSA and riboflavin were investigated in F68-alginate composite hydrogels. Results indicate that small molecule transport (represented by riboflavin) was not significantly hindered by F68 in homogeneously crosslinked hydrogels (up to an 11% decrease in loading capacity and 14% increase in effective diffusion coefficient, Deff), while protein transport in homogeneously crosslinked hydrogels (represented by BSA) was significantly affected (up to a 43% decrease in loading capacity and 40% increase in Deff). For inhomogeneously crosslinked hydrogels (CaCl2 or BaCl2 gelation), the Deff increased up to 50% and 83% for small molecule and proteins, respectively. Variation in the alginate gelation method was shown to affect transport through measurable changes in swelling ratio (30% decrease) and observable changes in crosslinking structure as well as up to a 3.6 and 11.8-fold difference in Deff for riboflavin and BSA, respectively. The change in protein transport properties is a product of mesh size restrictions (10–25 nm estimated by mechanical properties) and BSA-F68 interaction (DLS). Taken as a whole, these results show that incorporation of a nonionic surfactant at concentrations above the CMC can affect device functionality by impeding the transport of large biological molecules. PMID:21798381

Multiphoton imaging of myogenic differentiation in gelatin-based hydrogels as tissue engineering scaffolds.

PubMed

Kim, Min Jeong; Shin, Yong Cheol; Lee, Jong Ho; Jun, Seung Won; Kim, Chang-Seok; Lee, Yunki; Park, Jong-Chul; Lee, Soo-Hong; Park, Ki Dong; Han, Dong-Wook

2016-01-01

Hydrogels can serve as three-dimensional (3D) scaffolds for cell culture and be readily injected into the body. Recent advances in the image technology for 3D scaffolds like hydrogels have attracted considerable attention to overcome the drawbacks of ordinary imaging technologies such as optical and fluorescence microscopy. Multiphoton microscopy (MPM) is an effective method based on the excitation of two-photons. In the present study, C2C12 myoblasts differentiated in 3D gelatin hydroxyphenylpropionic acid (GHPA) hydrogels were imaged by using a custom-built multiphoton excitation fluorescence microscopy to compare the difference in the imaging capacity between conventional microscopy and MPM. The physicochemical properties of GHPA hydrogels were characterized by using scanning electron microscopy and Fourier-transform infrared spectroscopy. In addition, the cell viability and proliferation of C2C12 myoblasts cultured in the GHPA hydrogels were analyzed by using Live/Dead Cell and CCK-8 assays, respectively. It was found that C2C12 cells were well grown and normally proliferated in the hydrogels. Furthermore, the hydrogels were shown to be suitable to facilitate the myogenic differentiation of C2C12 cells incubated in differentiation media, which had been corroborated by MPM. It was very hard to get clear images from a fluorescence microscope. Our findings suggest that the gelatin-based hydrogels can be beneficially utilized as 3D scaffolds for skeletal muscle engineering and that MPM can be effectively applied to imaging technology for tissue regeneration.

A postoperative anti-adhesion barrier based on photoinduced imine-crosslinking hydrogel with tissue-adhesive ability.

PubMed

Yang, Yunlong; Liu, Xiaolin; Li, Yan; Wang, Yang; Bao, Chunyan; Chen, Yunfeng; Lin, Qiuning; Zhu, Linyong

2017-10-15

Postoperative adhesion is a serious complication that can further lead to morbidity and/or mortality. Polymer anti-adhesion barrier material provides an effective precaution to reduce the probability of postoperative adhesion. Clinical application requires these materials to be easily handled, biocompatible, biodegradable, and most importantly tissue adherent to provide target sites with reliable isolation. However, currently there is nearly no polymer barrier material that can fully satisfy these requirements. In this study, based on the photoinduced imine-crosslinking (PIC) reaction, we had developed a photo-crosslinking hydrogel (CNG hydrogel) that composed of o-nitrobenzyl alcohol (NB) modified carboxymethyl cellulose (CMC-NB) and glycol chitosan (GC) as an anti-adhesion barrier material. Under light irradiation, CMC-NB generated aldehyde groups which subsequently reacted with amino groups distributed on GC or tissue surface to form a hydrogel barrier that covalently attached to tissue surface. Rheological analysis demonstrated that CNG hydrogel (30mg/mL polymer content) could be formed in 30s upon light irradiation. Tissue adhesive tests showed that the tissue adhesive strength of CNG hydrogel (30mg/mL) was about 8.32kPa-24.65kPa which increased with increasing CMC-NB content in CNG hydrogel. Toxicity evaluation by L929 cells demonstrated that CNG hydrogel was cytocompatible. Furthermore, sidewall defect-cecum abrasion model of rat was employed to evaluate the postoperative anti-adhesion efficacy of CNG hydrogel. And a significantly reduction of tissue adhesion (20% samples with low score adhesion) was found in CNG hydrogel treated group, compared with control group (100% samples with high score adhesion). In addition, CNG hydrogel could be degraded in nearly 14days and showed no side effect on wound healing. These findings indicated that CNG hydrogel can effectively expanded the clinical treatments of postoperative tissue adhesion. In this study, a tissue adhesive photo-crosslinking hydrogel (CNG) was developed based on photo-induced imine crosslinking reaction (PIC) for postoperative anti-adhesion. CNG hydrogel showed the features of easy and convenient operation, fast and controllable gelation, suitable gel strength, good biocompatibility, and most importantly strong tissue adhesiveness. Therefore, it shows very high performance to prevent postoperative tissue adhesion. Overall, our study provides a more suitable hydrogel barrier material that can overcome the shortcomings of current barriers for clinical postoperative anti-adhesion. Copyright © 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Synthesis and characterization of psyllium-NVP based drug delivery system through radiation crosslinking polymerization

NASA Astrophysics Data System (ADS)

Singh, Baljit; Kumar, S.

2008-08-01

In order to develop the hydrogels meant for the drug delivery, we have prepared psyllium- N-vinylpyrrolidone (NVP) based hydrogels by radiation induced crosslinking. Polymers were characterized with SEMs, FTIR and swelling studies. Swelling of the hydrogels was studied as a function of monomer concentration, total radiation dose, temperature, pH and [NaCl] of the swelling medium. The swelling kinetics of the hydrogels and release dynamics of anticancer model drug (5-fluorouracil) from the hydrogels have been carried out for the evaluation of swelling and drug release mechanism. It has been observed that diffusion exponent ' n' have 0.8, 0.9, 0.8 and gel characteristics constant ' k' have 9.22 × 10 -3, 2.06 × 10 -3, 11.72 × 10 -3 values for the release of drug from the drug loaded hydrogels in distilled water, pH 2.2 buffer and pH 7.4 buffer, respectively. The present study shows that the release of drug from the hydrogels occurred through Non-Fickian diffusion mechanism.

Novel vaginal drug delivery system: deformable propylene glycol liposomes-in-hydrogel.

PubMed

Vanić, Željka; Hurler, Julia; Ferderber, Kristina; Golja Gašparović, Petra; Škalko-Basnet, Nataša; Filipović-Grčić, Jelena

2014-03-01

Deformable propylene glycol-containing liposomes (DPGLs) incorporating metronidazole or clotrimazole were prepared and evaluated as an efficient drug delivery system to improve the treatment of vaginal microbial infections. The liposome formulations were optimized based on sufficient trapping efficiencies for both drugs and membrane elasticity as a prerequisite for successful permeability and therapy. An appropriate viscosity for vaginal administration was achieved by incorporating the liposomes into Carbopol hydrogel. DPGLs were able to penetrate through the hydrogel network more rapidly than conventional liposomes. In vitro studies of drug release from the liposomal hydrogel under conditions simulating human treatment confirmed sustained and diffusion-based drug release. Characterization of the rheological and textural properties of the DPGL-containing liposomal hydrogels demonstrated that the incorporation of DPGLs alone had no significant influence on mechanical properties of hydrogels compared to controls. These results support the great potential of DPGL-in-hydrogel as an efficient delivery system for the controlled and sustained release of antimicrobial drugs in the vagina.

Injectable and body temperature sensitive hydrogels based on chitosan and hyaluronic acid for pH sensitive drug release.

PubMed

Zhang, Wei; Jin, Xin; Li, Heng; Zhang, Run-Run; Wu, Cheng-Wei

2018-04-15

Hydrogels based on chitosan/hyaluronic acid/β-sodium glycerophosphate demonstrate injectability, body temperature sensitivity, pH sensitive drug release and adhesion to cancer cell. The drug (doxorubicin) loaded hydrogel precursor solutions are injectable and turn to hydrogels when the temperature is increased to body temperature. The acidic condition (pH 4.00) can trigger the release of drug and the cancer cell (Hela) can adhere to the surface of the hydrogels, which will be beneficial for tumor site-specific administration of drug. The mechanical strength, the gelation temperature, and the drug release behavior can be tuned by varying hyaluronic acid content. The mechanisms were characterized using dynamic mechanical analysis, Fourier transform infrared spectroscopy, scanning electron microscopy and fluorescence microscopy. The carboxyl group in hyaluronic acid can form the hydrogen bondings with the protonated amine in chitosan, which promotes the increase of mechanical strength of the hydrogels and depresses the initial burst release of drug from the hydrogel. Copyright © 2018 Elsevier Ltd. All rights reserved.

Ionizing radiation in the field of hydrogels used for agriculture and medicine

NASA Astrophysics Data System (ADS)

Radoiu, M.; Martin, D.; Oproiu, C.; Toma, M.; Popescu, A. S.; Bestea, V.; Dragusin, M.; Moraru, R.; Calinescu, I.; Manea, A.

1999-01-01

Some hydrogel types, obtained by gamma ray and electron beam irradiation, such as homopolymers of acrylamide (pAA type), co-polymers of acrylamide and sodium acrylate (pAANA type), homo-polymers of sodium acrylate (pNA type) and homo-polymers of 2-hydroxyethylmethacrylate (pHEMA type), are presented. The effects of the solution's chemical composition, swelling medium nature, radiation absorbed dose and radiation absorbed dose rate upon the swelling degree and mechanical strength of pAA, pAANA, pNA types are discussed. For the pHEMA type, which are reinforced in the polyester network, the studies concerning the influence of the irradiation parameters and chemical composition upon the shape stability after swelling and surface's roughness are also discussed.

Soft Tissue Phantoms for Realistic Needle Insertion: A Comparative Study.

PubMed

Leibinger, Alexander; Forte, Antonio E; Tan, Zhengchu; Oldfield, Matthew J; Beyrau, Frank; Dini, Daniele; Rodriguez Y Baena, Ferdinando

2016-08-01

Phantoms are common substitutes for soft tissues in biomechanical research and are usually tuned to match tissue properties using standard testing protocols at small strains. However, the response due to complex tool-tissue interactions can differ depending on the phantom and no comprehensive comparative study has been published to date, which could aid researchers to select suitable materials. In this work, gelatin, a common phantom in literature, and a composite hydrogel developed at Imperial College, were matched for mechanical stiffness to porcine brain, and the interactions during needle insertions within them were analyzed. Specifically, we examined insertion forces for brain and the phantoms; we also measured displacements and strains within the phantoms via a laser-based image correlation technique in combination with fluorescent beads. It is shown that the insertion forces for gelatin and brain agree closely, but that the composite hydrogel better mimics the viscous nature of soft tissue. Both materials match different characteristics of brain, but neither of them is a perfect substitute. Thus, when selecting a phantom material, both the soft tissue properties and the complex tool-tissue interactions arising during tissue manipulation should be taken into consideration. These conclusions are presented in tabular form to aid future selection.

Biodegradable Cellulose-based Hydrogels: Design and Applications

PubMed Central

Sannino, Alessandro; Demitri, Christian; Madaghiele, Marta

2009-01-01

Hydrogels are macromolecular networks able to absorb and release water solutions in a reversible manner, in response to specific environmental stimuli. Such stimuli-sensitive behaviour makes hydrogels appealing for the design of ‘smart’ devices, applicable in a variety of technological fields. In particular, in cases where either ecological or biocompatibility issues are concerned, the biodegradability of the hydrogel network, together with the control of the degradation rate, may provide additional value to the developed device. This review surveys the design and the applications of cellulose-based hydrogels, which are extensively investigated due to the large availability of cellulose in nature, the intrinsic degradability of cellulose and the smart behaviour displayed by some cellulose derivatives.

Glutathione-Triggered Formation of a Fmoc-Protected Short Peptide-Based Supramolecular Hydrogel

PubMed Central

Shi, Yang; Wang, Jingyu; Wang, Huaimin; Hu, Yanhui; Chen, Xuemei; Yang, Zhimou

2014-01-01

A biocompatible method of glutathione (GSH) catalyzed disulfide bond reduction was used to form Fmoc-short peptide-based supramolecular hydrogels. The hydrogels could form in both buffer solution and cell culture medium containing 10% of Fetal Bovine Serum (FBS) within minutes. The hydrogel was characterized by rheology, transmission electron microscopy, and fluorescence emission spectra. Their potential in three dimensional (3D) cell culture was evaluated and the results indicated that the gel with a low concentration of the peptide (0.1 wt%) was suitable for 3D cell culture of 3T3 cells. This study provides an alternative candidate of supramolecular hydrogel for 3D cell culture and cell delivery. PMID:25222132

Synthesis and Characterization of Poly(Ethylene Glycol) Based Thermo-Responsive Hydrogels for Cell Sheet Engineering.

PubMed

Son, Kuk Hui; Lee, Jin Woo

2016-10-20

The swelling properties and thermal transition of hydrogels can be tailored by changing the hydrophilic-hydrophobic balance of polymer networks. Especially, poly( N -isopropylacrylamide) (PNIPAm) has received attention as thermo-responsive hydrogels for tissue engineering because its hydrophobicity and swelling property are transited around body temperature (32 °C). In this study, we investigated the potential of poly(ethylene glycol) diacrylate (PEGDA) as a hydrophilic co-monomer and crosslinker of PNIPAm to enhance biological properties of PNIPAm hydrogels. The swelling ratios, lower critical solution temperature (LCST), and internal pore structure of the synthesized p(NIPAm- co -PEGDA) hydrogels could be varied with changes in the molecular weight of PEGDA and the co-monomer ratios (NIPAm to PEGDA). We found that increasing the molecular weight of PEGDA showed an increase of pore sizes and swelling ratios of the hydrogels. In contrast, increasing the weight ratio of PEGDA under the same molecular weight condition increased the crosslinking density and decreased the swelling ratios of the hydrogels. Further, to evaluate the potential of these hydrogels as cell sheets, we seeded bovine chondrocytes on the p(NIPAm- co -PEGDA) hydrogels and observed the proliferation of the seed cells and their detachment as a cell sheet upon a decrease in temperature. Based on our results, we confirmed that p(NIPAm- co -PEGDA) hydrogels could be utilized as cell sheets with enhanced cell proliferation performance.

Soft contact lens biomaterials from bioinspired phospholipid polymers.

PubMed

Goda, Tatsuro; Ishihara, Kazuhiko

2006-03-01

Soft contact lens (SCL) biomaterials originated from the discovery of a poly(2-hydroxyethyl methacrylate) (poly[HEMA])-based hydrogel in 1960. Incorporation of hydrophilic polymers into poly(HEMA) hydrogels was performed in the 1970-1980s, which brought an increase in the equilibrium water content, leading to an enhancement of the oxygen permeability. Nowadays, the poly(HEMA)-based hydrogels have been applied in disposable SCL. At the same time, high oxygen-permeable silicone hydrogels were produced, which made it possible to continually wear SCL. Recently, numerous trials for improving the water wettability of silicone hydrogels have been performed. However, little attention has been paid to improving their anti-biofouling properties and biocompatibility. Since biomimetic phospholipid polymers possess excellent anti-biofouling properties and biocompatibility they have the potential to play a valuable role in the surface modification of the silicone hydrogel. The representative phospholipid polymers containing a 2-methacryloyloxyethyl phosphorylcholine (MPC) unit suppressed nonspecific protein adsorption, increased cell compatibility and contributed to blood compatible biomaterials. The MPC polymer coating on the silicone hydrogel improved its water wettability and biocompatibility, while maintaining high oxygen permeability compared with the original silicone hydrogel. Furthermore, the newly prepared phospholipid-type intermolecular crosslinker made it possible to synthesize a 100% phospholipid polymer hydrogel that can enhance the anti-biofouling properties and biocompatibility. In this review, the authors discuss how polymer hydrogels should be designed in order to obtain a biocompatible SCL and future perspectives.

pH-sensitive Itaconic acid based polymeric hydrogels for dye removal applications.

PubMed

Sakthivel, M; Franklin, D S; Guhanathan, S

2016-12-01

A series of Itaconic Acid (IA) based pH-sensitive polymeric hydrogels were synthesized by condensation polymerization of Itaconic Acid (IA) with Ethylene Glycol (EG) in the presence of an acid medium resulted into pre-polymer. Further, pre-polymer were co-polymerized with Acrylic Acid (AA) through free radical polymerization using Potassium persulphate (KPS). The structural and surface morphological characterizations of the synthesized hydrogels were studied using FT-IR spectroscopy and Scanning Electron Microscope (SEM) respectively. The swelling and swelling equilibrium were performed at varies pH (4.0-10.0). Further, the effects of IA, EG and AA on swelling properties have also been investigated. Thermal stability of synthesized hydrogels have been investigated by TGA, DTA and DSC. The synthesized hydrogels have shown good ability to uptake a Cationic dye. The Methylene blue has been chosen as a model cationic dye. The results of dye removal using IA hydrogels found to have excellent dye removal capacity. Such kind of IA based hydrogels may be recommended for eco-friendly environmental application. viz., removal of dyes and metal ions and sewage water treatment, purification of water etc. Copyright © 2015 Elsevier Inc. All rights reserved.

A facile prestrain-stick-release assembly of stretchable supercapacitors based on highly stretchable and sticky hydrogel electrolyte

NASA Astrophysics Data System (ADS)

Tang, Qianqiu; Chen, Mingming; Wang, Gengchao; Bao, Hua; Saha, Petr

2015-06-01

A facile prestrain-stick-release assembly strategy for the stretchable supercapacitor device is developed based on a novel Na2SO4-aPUA/PAAM hydrogel electrolyte, saving the stretchable rubber base conventionally used. The Na2SO4-aPUA/PAAM hydrogel electrolyte exhibits high stretchability (>1000%), electrical conductivity (0.036 S cm-1) and stickiness. Due to the unique features of the hydrogel electrolyte, the carbon nanotube@MnO2 film electrodes can be firmly stuck to two sides of the prestrained hydrogel electrolyte. Then, by releasing the hydrogel electrolyte, homogenous buckles are formed for the film electrodes to get a full stretchable supercapacitor device. Besides, the high stickiness of the hydrogel electrolyte ensures its strong adhesion with the film electrodes, facilitating ion and electronic transfer of the supercapacitor. As a result, excellent electrochemical performance is achieved with the specific capacitance of 478.6 mF cm-2 at 0.5 mA cm-2 (corresponding to 201.1 F g-1) and capacitance retention of 91.5% after 3000 charging-discharging cycles under 150% strain, which is the best for the stretchable supercapacitors.

3D Printing of Thermo-Responsive Methylcellulose Hydrogels for Cell-Sheet Engineering.

PubMed

Cochis, Andrea; Bonetti, Lorenzo; Sorrentino, Rita; Contessi Negrini, Nicola; Grassi, Federico; Leigheb, Massimiliano; Rimondini, Lia; Farè, Silvia

2018-04-10

A possible strategy in regenerative medicine is cell-sheet engineering (CSE), i.e., developing smart cell culture surfaces from which to obtain intact cell sheets (CS). The main goal of this study was to develop 3D printing via extrusion-based bioprinting of methylcellulose (MC)-based hydrogels. Hydrogels were prepared by mixing MC powder in saline solutions (Na₂SO₄ and PBS). MC-based hydrogels were analyzed to investigate the rheological behavior and thus optimize the printing process parameters. Cells were tested in vitro on ring-shaped printed hydrogels; bulk MC hydrogels were used for comparison. In vitro tests used murine embryonic fibroblasts (NIH/3T3) and endothelial murine cells (MS1), and the resulting cell sheets were characterized analyzing cell viability and immunofluorescence. In terms of CS preparation, 3D printing proved to be an optimal approach to obtain ring-shaped CS. Cell orientation was observed for the ring-shaped CS and was confirmed by the degree of circularity of their nuclei: cell nuclei in ring-shaped CS were more elongated than those in sheets detached from bulk hydrogels. The 3D printing process appears adequate for the preparation of cell sheets of different shapes for the regeneration of complex tissues.

Elastin Based Cell-laden Injectable Hydrogels with Tunable Gelation, Mechanical and Biodegradation Properties

PubMed Central

Fathi, Ali; Mithieux, Suzanne M.; Wei, Hua; Chrzanowski, Wojciech; Valtchev, Peter; Weiss, Anthony S.; Dehghani, Fariba

2015-01-01

Injectable hydrogels made from extracellular matrix proteins such as elastin show great promise for various biomedical applications. Use of cytotoxic reagents, fixed gelling behavior, and lack of mechanical strength in these hydrogels are the main associated drawbacks. The aim of this study was to develop highly cytocompatible and injectable elastin-based hydrogels with alterable gelation characteristics, favorable mechanical properties and structural stability for load bearing applications. A thermoresponsive copolymer, poly(N-isopropylacrylamide-co-polylactide-2-hydroxyethyl methacrylate-co-oligo(ethylene glycol)monomethyl ether methacrylate, was functionalized with succinimide ester groups by incorporating N-acryloxysuccinimide monomer. These ester groups were exploited to covalently bond this polymer, denoted as PNPHO, to different proteins with primary amine groups such as α-elastin in aqueous media. The incorporation of elastin through covalent bond formation with PNPHO promotes the structural stability, mechanical properties and live cell proliferation within the structure of hydrogels. Our results demonstrated that elastin-co-PNPHO solutions were injectable through fine gauge needles and converted to hydrogels in situ at 37 °C in the absence of any crosslinking reagent. By altering PNPHO content, the gelling time of these hydrogels can be finely tuned within the range of 2 to 15 min to ensure compatibility with surgical requirements. In addition, these hydrogels exhibited compression moduli in the range of 40 to 145 kPa, which are substantially higher than those of previously developed elastin-based hydrogels. These hydrogels were highly stable in the physiological environment with the evidence of 10 wt% mass loss in 30 days of incubation in a simulated environment. This class of hydrogels is in vivo bioabsorbable due to the gradual increase of the lower critical solution temperature of the copolymer to above 37 °C due to the cleavage of polylactide from the PNPHO copolymer. Moreover, our results demonstrated that more than 80% of cells encapsulated in these hydrogels remained viable, and the number of encapsulated cells increased for at least 5 days. These unique properties mark elastin-co-PNHPO hydrogels as favorable candidates for a broad range of tissue engineering applications. PMID:24731705

Biocompatible and biodegradable dual-drug release system based on silk hydrogel containing silk nanoparticles.

PubMed

Numata, Keiji; Yamazaki, Shoya; Naga, Naofumi

2012-05-14

We developed a facile and quick ethanol-based method for preparing silk nanoparticles and then fabricated a biodegradable and biocompatible dual-drug release system based on silk nanoparticles and the molecular networks of silk hydrogels. Model drugs incorporated in the silk nanoparticles and silk hydrogels showed fast and constant release, respectively, indicating successful dual-drug release from silk hydrogel containing silk nanoparticles. The release behaviors achieved by this dual-drug release system suggest to be regulated by physical properties (e.g., β-sheet contents and size of the silk nanoparticles and network size of the silk hydrogels), which is an important advantage for biomedical applications. The present silk-based system for dual-drug release also demonstrated no significant cytotoxicity against human mesenchymal stem cells (hMSCs), and thus, this silk-based dual-drug release system has potential as a versatile and useful new platform of polymeric materials for various types of dual delivery of bioactive molecules.

Injectable bioadhesive hydrogels with innate antibacterial properties

NASA Astrophysics Data System (ADS)

Giano, Michael C.; Ibrahim, Zuhaib; Medina, Scott H.; Sarhane, Karim A.; Christensen, Joani M.; Yamada, Yuji; Brandacher, Gerald; Schneider, Joel P.

2014-06-01

Surgical site infections cause significant postoperative morbidity and increased healthcare costs. Bioadhesives used to fill surgical voids and support wound healing are typically devoid of antibacterial activity. Here we report novel syringe-injectable bioadhesive hydrogels with inherent antibacterial properties prepared from mixing polydextran aldehyde and branched polyethylenimine. These adhesives kill both Gram-negative and Gram-positive bacteria, while sparing human erythrocytes. An optimal composition of 2.5 wt% oxidized dextran and 6.9 wt% polyethylenimine sets within seconds forming a mechanically rigid (~\

Self-healing polysaccharide-based hydrogels as injectable carriers for neural stem cells

PubMed Central

Wei, Zhao; Zhao, Jingyi; Chen, Yong Mei; Zhang, Pengbo; Zhang, Qiqing

2016-01-01

Self-healing injectable hydrogels can be formulated as three-dimensional carriers for the treatment of neurological diseases with desirable advantages, such as avoiding the potential risks of cell loss during injection, protecting cells from the shearing force of injection. However, the demands for biocompatible self-healing injectable hydrogels to meet above requirements and to promote the differentiation of neural stem cells (NSCs) into neurons remain a challenge. Herein, we developed a biocompatible self-healing polysaccharide-based hydrogel system as a novel injectable carrier for the delivery of NSCs. N-carboxyethyl chitosan (CEC) and oxidized sodium alginate (OSA) are the main backbones of the hydrogel networks, denoted as CEC-l-OSA hydrogel (“l” means “linked-by”). Owing to the dynamic imine cross-links formed by a Schiff reaction between amino groups on CEC and aldehyde groups on OSA, the hydrogel possesses the ability to self-heal into a integrity after being injected from needles under physiological conditions. The CEC-l-OSA hydrogel in which the stiffness mimicking nature brain tissues (100~1000 Pa) can be finely tuned to support the proliferation and neuronal differentiation of NSCs. The multi-functional, injectable, and self-healing CEC-l-OSA hydrogels hold great promises for NSC transplantation and further treatment of neurological diseases. PMID:27897217

Chitosan-based thermosensitive hydrogel as a promising ocular drug delivery system: preparation, characterization, and in vivo evaluation.

PubMed

Chen, Xingwei; Li, Xinru; Zhou, Yanxia; Wang, Xiaoning; Zhang, Yanhui; Fan, Yating; Huang, Yanqing; Liu, Yan

2012-11-01

The purpose of this study was to evaluate the feasibility of in situ thermosensitive hydrogel based on chitosan in combination with disodium α-d-Glucose 1-phosphate (DGP) for ocular drug delivery system. Aqueous solution of chitosan/DGP underwent sol-gel transition as temperature increased which was flowing sol at room temperature and then turned into non-flowing hydrogel at physiological temperature. The properties of gels were characterized regarding gelation time, gelation temperature, and morphology. The sol-to-gel phase transition behaviors were affected by the concentrations of chitosan, DGP and the model drug levocetirizine dihydrochloride (LD). The developed hydrogel presented a characteristic of a rapid release at the initial period followed by a sustained release and remarkably enhanced the cornea penetration of LD. The results of ocular irritation demonstrated the excellent ocular tolerance of the hydrogel. The ocular residence time for the hydrogel was significantly prolonged compared with eye drops. The drug-loaded hydrogel produced more effective anti-allergic conjunctivitis effects compared with LD aqueous solution. These results showed that the chitosan/DGP thermosensitive hydrogel could be used as an ideal ocular drug delivery system in terms of the suitable sol-gel transition temperature, mild pH environment in the hydrogel as well as the organic solvent free.

Self-healing polysaccharide-based hydrogels as injectable carriers for neural stem cells

NASA Astrophysics Data System (ADS)

Wei, Zhao; Zhao, Jingyi; Chen, Yong Mei; Zhang, Pengbo; Zhang, Qiqing

2016-11-01

Self-healing injectable hydrogels can be formulated as three-dimensional carriers for the treatment of neurological diseases with desirable advantages, such as avoiding the potential risks of cell loss during injection, protecting cells from the shearing force of injection. However, the demands for biocompatible self-healing injectable hydrogels to meet above requirements and to promote the differentiation of neural stem cells (NSCs) into neurons remain a challenge. Herein, we developed a biocompatible self-healing polysaccharide-based hydrogel system as a novel injectable carrier for the delivery of NSCs. N-carboxyethyl chitosan (CEC) and oxidized sodium alginate (OSA) are the main backbones of the hydrogel networks, denoted as CEC-l-OSA hydrogel (“l” means “linked-by”). Owing to the dynamic imine cross-links formed by a Schiff reaction between amino groups on CEC and aldehyde groups on OSA, the hydrogel possesses the ability to self-heal into a integrity after being injected from needles under physiological conditions. The CEC-l-OSA hydrogel in which the stiffness mimicking nature brain tissues (100~1000 Pa) can be finely tuned to support the proliferation and neuronal differentiation of NSCs. The multi-functional, injectable, and self-healing CEC-l-OSA hydrogels hold great promises for NSC transplantation and further treatment of neurological diseases.

Gene Therapy Vectors with Enhanced Transfection Based on Hydrogels Modified with Affinity Peptides

PubMed Central

Shepard, Jaclyn A.; Wesson, Paul J.; Wang, Christine E.; Stevans, Alyson C.; Holland, Samantha J.; Shikanov, Ariella; Grzybowski, Bartosz A.; Shea, Lonnie D.

2011-01-01

Regenerative strategies for damaged tissue aim to present biochemical cues that recruit and direct progenitor cell migration and differentiation. Hydrogels capable of localized gene delivery are being developed to provide a support for tissue growth, and as a versatile method to induce the expression of inductive proteins; however, the duration, level, and localization of expression isoften insufficient for regeneration. We thus investigated the modification of hydrogels with affinity peptides to enhance vector retention and increase transfection within the matrix. PEG hydrogels were modified with lysine-based repeats (K4, K8), which retained approximately 25% more vector than control peptides. Transfection increased 5- to 15-fold with K8 and K4 respectively, over the RDG control peptide. K8- and K4-modified hydrogels bound similar quantities of vector, yet the vector dissociation rate was reduced for K8, suggesting excessive binding that limited transfection. These hydrogels were subsequently applied to an in vitro co-culture model to induce NGF expression and promote neurite outgrowth. K4-modified hydrogels promoted maximal neurite outgrowth, likely due to retention of both the vector and the NGF. Thus, hydrogels modified with affinity peptides enhanced vector retention and increased gene delivery, and these hydrogels may provide a versatile scaffold for numerous regenerative medicine applications. PMID:21514659

Facile synthesis of degradable and electrically conductive polysaccharide hydrogels.

PubMed

Guo, Baolin; Finne-Wistrand, Anna; Albertsson, Ann-Christine

2011-07-11

Degradable and electrically conductive polysaccharide hydrogels (DECPHs) have been synthesized by functionalizing polysaccharide with conductive aniline oligomers. DECPHs based on chitosan (CS), aniline tetramer (AT), and glutaraldehyde were obtained by a facile one-pot reaction by using the amine group of CS and AT under mild conditions, which avoids the multistep reactions and tedious purification involved in the synthesis of degradable conductive hydrogels in our previous work. Interestingly, these one-pot hydrogels possess good film-forming properties, electrical conductivity, and a pH-sensitive swelling behavior. The chemical structure and morphology before and after swelling of the hydrogels were verified by FT-IR, NMR, and SEM. The conductivity of the hydrogels was tuned by adjusting the content of AT. The swelling ratio of the hydrogels was altered by the content of tetraaniline and cross-linker. The hydrogels underwent slow degradation in a buffer solution. The hydrogels obtained by this facile approach provide new possibilities in biomedical applications, for example, biodegradable conductive hydrogels, films, and scaffolds for cardiovascular tissue engineering and controlled drug delivery.

Behavior of POP-calcium carbonate hydrogel as bone substitute with controlled release capability: a study in rat.

PubMed

Dewi, Anne Handrini; Ana, Ika Dewi; Wolke, Joop; Jansen, John

2015-10-01

Gypsum or calcium sulfate (CS) or plaster of Paris (POP) is considered as a fast degradable material that usually resorbs before the bone defect area is completely filled by new bone. In this study, the incorporation of CaCO3 hydrogel into POP in different compositions was proposed to enhance the bone biological activity of POP and to decrease its degradability. The mechanical and degradation properties of the various materials were characterized by in vitro analysis. Subsequently, the materials were inserted into cylindrically sized bone defects as created into the femoral condyle of rats and left in situ for 1, 4, and 8 weeks. Histological analysis of the retrieved specimens indicated that the addition of CaCO3 hydrogel into POP increased bone formation, angiogenesis and collagen density and resulted into faster bone formation and maturation. It was also confirmed that the degradation rate of the POP decreased by the addition of CaCO3 hydrogel. The in vivo findings did corroborate with the in vitro analysis. In conclusion, the incorporation of CaCO3 hydrogel provides a promising technology to improve the properties of POP, the oldest biomaterial used for bone grafting. © 2015 Wiley Periodicals, Inc.

High-resolution synchrotron X-ray analysis of bioglass-enriched hydrogels.

PubMed

Gorodzha, Svetlana; Douglas, Timothy E L; Samal, Sangram K; Detsch, Rainer; Cholewa-Kowalska, Katarzyna; Braeckmans, Kevin; Boccaccini, Aldo R; Skirtach, Andre G; Weinhardt, Venera; Baumbach, Tilo; Surmeneva, Maria A; Surmenev, Roman A

2016-05-01

Enrichment of hydrogels with inorganic particles improves their suitability for bone regeneration by enhancing their mechanical properties, mineralizability, and bioactivity as well as adhesion, proliferation, and differentiation of bone-forming cells, while maintaining injectability. Low aggregation and homogeneous distribution maximize particle surface area, promoting mineralization, cell-particle interactions, and homogenous tissue regeneration. Hence, determination of the size and distribution of particles/particle agglomerates in the hydrogel is desirable. Commonly used techniques have drawbacks. High-resolution techniques (e.g., SEM) require drying. Distribution in the dry state is not representative of the wet state. Techniques in the wet state (histology, µCT) are of lower resolution. Here, self-gelling, injectable composites of Gellan Gum (GG) hydrogel and two different types of sol-gel-derived bioactive glass (bioglass) particles were analyzed in the wet state using Synchrotron X-ray radiation, enabling high-resolution determination of particle size and spatial distribution. The lower detection limit volume was 9 × 10(-5) mm(3) . Bioglass particle suspensions were also studied using zeta potential measurements and Coulter analysis. Aggregation of bioglass particles in the GG hydrogels occurred and aggregate distribution was inhomogeneous. Bioglass promoted attachment of rat mesenchymal stem cells (rMSC) and mineralization. © 2016 Wiley Periodicals, Inc.

Injectable glycosaminoglycan-protein nano-complex in semi-interpenetrating networks: A biphasic hydrogel for hyaline cartilage regeneration.

PubMed

Radhakrishnan, Janani; Subramanian, Anuradha; Sethuraman, Swaminathan

2017-11-01

Articular hyaline cartilage regeneration remains challenging due to its less intrinsic reparability. The study develops injectable biphasic semi-interpenetrating polymer networks (SIPN) hydrogel impregnated with chondroitin sulfate (ChS) nanoparticles for functional cartilage restoration. ChS loaded zein nanoparticles (∼150nm) prepared by polyelectrolyte-protein complexation were interspersed into injectable SIPNs developed by blending alginate with poly(vinyl alcohol) and calcium crosslinking. The hydrogel exhibited interconnected porous microstructure (39.9±5.8μm pore diameter, 57.7±5.9% porosity), 92% swellability and >350Pa elastic modulus. Primary chondrocytes compatibility, chondrocyte-matrix interaction with cell-cell clustering and spheroidal morphology was demonstrated in ChS loaded hydrogel and long-term (42days) proliferation was also determined. Higher fold expression of cartilage-specific genes sox9, aggrecan and collagen-II was observed in ChS loaded hydrogel while exhibiting poor expression of collagen-I. Immunoblotting of aggregan and collagen II demonstrate favorable positive influence of ChS on chondrocytes. Thus, the injectable biphasic SIPNs could be promising composition-mimetic substitute for cartilage restoration at irregular defects. Copyright © 2017 Elsevier Ltd. All rights reserved.

Micromechanical model of biphasic biomaterials with internal adhesion: Application to nanocellulose hydrogel composites.

PubMed

Bonilla, Mauricio R; Lopez-Sanchez, P; Gidley, M J; Stokes, J R

2016-01-01

The mechanical properties of hydrated biomaterials are non-recoverable upon unconfined compression if adhesion occurs between the structural components in the material upon fluid loss and apparent plastic behaviour. We explore these micromechanical phenomena by introducing an aggregation force and a critical yield pressure into the constitutive biphasic formulation for transversely isotropic tissues. The underlying hypothesis is that continual fluid pressure build-up during compression temporarily supresses aggregation. Once compression stops and the pressure falls below some critical value, internal aggregation occurs over a time scale comparable to the poroelastic time. We demonstrate this model by predicting the mechanical response of bacterial nanocellulose hydrogel composites, which are promising biomaterials and a structural mimetic for the plant cell wall. Cross-linking of cellulose by xyloglucan creates an extensional resistance and substantially increases the compressive modulus under large compression and densification. In comparison, incorporating non-crosslinking arabinoxylan into the hydrogel has little effect on its mechanics at the strain rates investigated. These results assist in elucidating the mechanical role of these polysaccharides in the complex plant cell wall structure. They also suggest xyloglucan is a suitable candidate to tailor the stiffness of nanocellulose hydrogels in biomaterial design, which includes modulating cell-adhesion in tissue engineering applications. The model and overall approach may be utilised to characterise and design a myriad of biomaterials and mammalian tissues, particularly those with a fibrillar structure. The mechanical properties of hydrated biomaterials can be non-recoverable upon compression due to increased adhesion occurring between the structural components in the material. Cellulose-hemicellulose composite hydrogels constitute a classical example of this phenomenon, since fibres can freely re-orient and adhere upon fluid loss to produce significant variations in the mechanical response to compression. Here, we model their micromechanics by introducing an aggregation force and a critical yield pressure into the constitutive formulation for transversely isotropic biphasic materials. The resulting model is easy to implement for routine characterization of this type of hydrated biomaterials through unconfined compression testing and produces physically meaningful and reproducible mechanical parameters. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Gradient nano-engineered in situ forming composite hydrogel for osteochondral regeneration.

PubMed

Radhakrishnan, Janani; Manigandan, Amrutha; Chinnaswamy, Prabu; Subramanian, Anuradha; Sethuraman, Swaminathan

2018-04-01

Fabrication of anisotropic osteochondral-mimetic scaffold with mineralized subchondral zone and gradient interface remains challenging. We have developed an injectable semi-interpenetrating network hydrogel construct with chondroitin sulfate nanoparticles (ChS-NPs) and nanohydroxyapatite (nHA) (∼30-90 nm) in chondral and subchondral hydrogel zones respectively. Mineralized subchondral hydrogel exhibited significantly higher osteoblast proliferation and alkaline phosphatase activity (p < 0.05). Osteochondral hydrogel exhibited interconnected porous structure and spatial variation with gradient interface of nHA and ChS-NPs. Microcomputed tomography (μCT) demonstrated nHA gradation while rheology showed predominant elastic modulus (∼930 Pa) at the interface. Co-culture of osteoblasts and chondrocytes in gradient hydrogels showed layer-specific retention of cells and cell-cell interaction at the interface. In vivo osteochondral regeneration by biphasic (nHA or ChS) and gradient (nHA + ChS) hydrogels was compared with control using rabbit osteochondral defect after 3 and 8 weeks. Complete closure of defect was observed in gradient (8 weeks) while defect remained in other groups. Histology demonstrated collagen and glycosaminoglycan deposition in neo-matrix and presence of hyaline cartilage-characteristic matrix, chondrocytes and osteoblasts. μCT showed mineralized neo-tissue formation, which was confined within the defect with higher bone mineral density in gradient (chondral: 0.42 ± 0.07 g/cc, osteal: 0.64 ± 0.08 g/cc) group. Further, biomechanical push-out studies showed significantly higher load for gradient group (378 ± 56 N) compared to others. Thus, the developed nano-engineered gradient hydrogel enhanced hyaline cartilage regeneration with subchondral bone formation and lateral host-tissue integration. Copyright © 2018 Elsevier Ltd. All rights reserved.

Mineralization behavior and interface properties of BG-PVA/bone composite implants in simulated body fluid.

PubMed

Ma, Yanxuan; Zheng, Yudong; Huang, Xiaoshan; Xi, Tingfei; Lin, Xiaodan; Han, Dongfei; Song, Wenhui

2010-04-01

Due to the non-bioactivity and poor conjunction performance of present cartilage prostheses, the main work here is to develop the bioactive glass-polyvinyl alcohol hydrogel articular cartilage/bone (BG-PVA/bone) composite implants. The essential criterion for a biomaterial to bond with living bone is well-matched mechanical properties as well as biocompatibility and bioactivity. In vitro studies on the formation of a surface layer of carbonate hydroxyl apatite (HCA) and the corresponding variation of the properties of biomaterials are imperative for their clinical application. In this paper, the mineralization behavior and variation of the interface properties of BG-PVA/bone composites were studied in vitro by using simulated body fluid (SBF). The mineralization and HCA layer formed on the interface between the BG-PVA hydrogel and bone in SBF could provide the composites with bioactivity and firmer combination. The compression property, shear strength and interface morphology of BG-PVA/bone composite implants varying with the immersion time in SBF were characterized. Also, the influence laws of the immersion time, content of BG in the composites and aperture of bones to the mineralization behavior and interface properties were investigated. The good mineralization behavior and enhanced conjunction performance of BG-PVA/bone composites demonstrated that this kind of composite implant might be more appropriate cartilage replacements.

Formulation and evaluation of microemulsion-based hydrogel for topical delivery

PubMed Central

Sabale, Vidya; Vora, Sejal

2012-01-01

Background: The purpose of this study was to develop microemulsion-based hydrogel formulation for topical delivery of bifonazole with an objective to increase the solubility and skin permeability of the drug. Materials and Methods: Oleic acid was screened as the oil phase of microemulsions, due to a good solubilizing capacity of the microemulison systems. The pseudo-ternary phase diagrams for microemulsion regions were constructed using oleic acid as the oil, Tween 80 as the surfactant and isopropyl alcohol (IPA) as the cosurfactant. Various microemulsion formulations were prepared and optimized by 32 factorial design on the basis of percentage (%) transmittance, globule size, zeta potential, drug release, and skin permeability. The abilities of various microemulsions to deliver bifonazole through the skin were evaluated ex vivo using Franz diffusion cells fitted with rat skins. The Hydroxy Propyl Methyl Cellulose (HPMC) K100 M as a gel matrix was used to construct the microemulsion-based hydrogel for improving the viscosity of microemulsion for topical administration. The optimized microemulsion-based hydrogel was evaluated for viscosity, spreadability, skin irritancy, skin permeability, stability, and antifungal activity by comparing it with marketed bifonazole cream. Results: The mechanism of drug release from microemulsion-based hydrogel was observed to follow zero order kinetics. The studied optimized microemulsion-based hydrogel showed a good stability over the period of 3 months. Average globule size of optimized microemulsion (F5) was found to be 18.98 nm, zeta potential was found to be -5.56 mv, and permeability of drug from microemulsion within 8 h was observed 84%. The antifungal activity of microemulsion-based hydrogel was found to be comparable with marketed cream. Conclusion: The results indicate that the studied microemulsion-based hydrogel (F5) has a potential for sustained action of drug release and it may act as promising vehicle for topical delivery of ibuprofen. PMID:23373005