Fabrication of elastomeric silk fibers.

Science.gov (United States)

Bradner, Sarah A; Partlow, Benjamin P; Cebe, Peggy; Omenetto, Fiorenzo G; Kaplan, David L

2017-09-01

Methods to generate fibers from hydrogels, with control over mechanical properties, fiber diameter, and crystallinity, while retaining cytocompatibility and degradability, would expand options for biomaterials. Here, we exploited features of silk fibroin protein for the formation of tunable silk hydrogel fibers. The biological, chemical, and morphological features inherent to silk were combined with elastomeric properties gained through enzymatic crosslinking of the protein. Postprocessing via methanol and autoclaving provided tunable control of fiber features. Mechanical, optical, and chemical analyses demonstrated control of fiber properties by exploiting the physical cross-links, and generating double network hydrogels consisting of chemical and physical cross-links. Structure and chemical analyses revealed crystallinity from 30 to 50%, modulus from 0.5 to 4 MPa, and ultimate strength 1-5 MPa depending on the processing method. Fabrication and postprocessing combined provided fibers with extensibility from 100 to 400% ultimate strain. Fibers strained to 100% exhibited fourth order birefringence, revealing macroscopic orientation driven by chain mobility. The physical cross-links were influenced in part by the drying rate of fabricated materials, where bound water, packing density, and microstructural homogeneity influenced cross-linking efficiency. The ability to generate robust and versatile hydrogel microfibers is desirable for bottom-up assembly of biological tissues and for broader biomaterial applications. © 2017 Wiley Periodicals, Inc.

Strong composite films with layered structures prepared by casting silk fibroin-graphene oxide hydrogels

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Huang, Liang; Li, Chun; Yuan, Wenjing; Shi, Gaoquan

2013-04-01

Composite films of graphene oxide (GO) sheets and silk fibroin (SF) with layered structures have been prepared by facile solution casting of SF-GO hydrogels. The as-prepared composite film containing 15% (by weight, wt%) of SF shows a high tensile strength of 221 +/- 16 MPa and a failure strain of 1.8 +/- 0.4%, which partially surpass those of natural nacre. Particularly, this composite film also has a high modulus of 17.2 +/- 1.9 GPa. The high mechanical properties of this composite film can be attributed to its high content of GO (85 wt%), compact layered structure and the strong hydrogen bonding interaction between SF chains and GO sheets.Composite films of graphene oxide (GO) sheets and silk fibroin (SF) with layered structures have been prepared by facile solution casting of SF-GO hydrogels. The as-prepared composite film containing 15% (by weight, wt%) of SF shows a high tensile strength of 221 +/- 16 MPa and a failure strain of 1.8 +/- 0.4%, which partially surpass those of natural nacre. Particularly, this composite film also has a high modulus of 17.2 +/- 1.9 GPa. The high mechanical properties of this composite film can be attributed to its high content of GO (85 wt%), compact layered structure and the strong hydrogen bonding interaction between SF chains and GO sheets. Electronic supplementary information (ESI) available: XPS spectrum of the SF-GO hybrid film, SEM images of lyophilized GO dispersion and the failure surface of GO film. See DOI: 10.1039/c3nr00196b

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

Science.gov (United States)

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.

Dilute self-healing hydrogels of silk-collagen-like block copolypeptides at neutral pH

NARCIS (Netherlands)

Golinska, M.D.; Wlodarczyk-Biegun, M.K.; Werten, M.W.T.; Cohen Stuart, M.A.; Wolf, de F.A.; Vries, de R.J.

2014-01-01

We report on self-healing, pH-responsive hydrogels that are entirely protein-based. The protein is a denovo designed recombinant triblock polypeptide of 66 kg/mol consisting of a silk-like middle block (GAGAGAGH)48, flanked by two long collagen-inspired hydrophilic random coil side blocks. The

Applicability of biotechnologically produced insect silks.

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Herold, Heike M; Scheibel, Thomas

2017-09-26

Silks are structural proteins produced by arthropods. Besides the well-known cocoon silk, which is produced by larvae of the silk moth Bombyx mori to undergo metamorphosis inside their silken shelter (and which is also used for textile production by men since millennia), numerous further less known silk-producing animals exist. The ability to produce silk evolved multiple independent times during evolution, and the fact that silk was subject to convergent evolution gave rise to an abundant natural diversity of silk proteins. Silks are used in air, under water, or like honey bee silk in the hydrophobic, waxen environment of the bee hive. The good mechanical properties of insect silk fibres together with their non-toxic, biocompatible, and biodegradable nature renders these materials appealing for both technical and biomedical applications. Although nature provides a great diversity of material properties, the variation in quality inherent in materials from natural sources together with low availability (except from silkworm silk) impeded the development of applications of silks. To overcome these two drawbacks, in recent years, recombinant silks gained more and more interest, as the biotechnological production of silk proteins allows for a scalable production at constant quality. This review summarises recent developments in recombinant silk production as well as technical procedures to process recombinant silk proteins into fibres, films, and hydrogels.

Behaviour of human mesenchymal stem cells on a polyelectrolyte-modified HEMA hydrogel for silk-based ligament tissue engineering.

Science.gov (United States)

Bosetti, M; Boccafoschi, F; Calarco, A; Leigheb, M; Gatti, S; Piffanelli, V; Peluso, G; Cannas, M

2008-01-01

The aim of this study was to design a functional bio-engineered material to be used as scaffold for autologous mesenchymal stem cells in ligament tissue engineering. Polyelectrolyte modified HEMA hydrogel (HEMA-co-METAC), applied as coating on silk fibroin fibres, has been formulated in order to take advantage of the biocompatibility of the polyelectrolyte by increasing its mechanical properties with silk fibres. Human bone marrow mesenchymal stem cells behaviour on such reinforced polyelectrolyte has been studied by evaluating cell morphology, cell number, attachment, spreading and proliferation together with collagen matrix production and its mRNA expression. Silk fibroin fibres matrices with HEMA-co-METAC coating exhibited acceptable mechanical behaviour compared to the natural ligament, good human mesenchymal stem cell adhesion and with mRNA expression studies higher levels of collagen types I and III expression when compared to control cells on polystyrene. These data indicate high expression of mRNA for proteins responsible for the functional characteristics of the ligaments and suggest a potential for use of this biomaterial in ligament tissue-engineering applications.

Preparation of wound dressing of polyvinyl alcohol/silk fibroin hydrogels by gamma radiation

International Nuclear Information System (INIS)

Kewsuwan, Prartana; Pongpat, Suchada; Sonsuk, Manit; Pongpat, Suchada

2004-10-01

Poly vinylalcohol/silk fibroin (PVA/SF) hydrogels were prepared by γ-radiation. The preparation conditions such as absorbed doses and PVA/SF concentrations were investigated. When exposed to γ -radiation, PVA/SF was crosslinked to yield high water absorption materials with water content of 100 - 1000% of their dried weight depending on the preparation conditions. The crosslinked density seems to be the main factor governing the swelling of these gels. The swelling behaviors in NaCl aqueous solutions were also investigated. The swelling of PVA/SF hydrogels decreases when exposed to electrolyte solution. With an increase of absorbed dose, the gel fraction of PVA/SF increases

Fabrication and Mechanical Characterization of Hydrogel Infused Network Silk Scaffolds

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Lakshminath Kundanati

2016-09-01

Full Text Available Development and characterization of porous scaffolds for tissue engineering and regenerative medicine is of great importance. In recent times, silk scaffolds were developed and successfully tested in tissue engineering and drug release applications. We developed a novel composite scaffold by mechanical infusion of silk hydrogel matrix into a highly porous network silk scaffold. The mechanical behaviour of these scaffolds was thoroughly examined for their possible use in load bearing applications. Firstly, unconfined compression experiments show that the denser composite scaffolds displayed significant enhancement in the elastic modulus as compared to either of the components. This effect was examined and further explained with the help of foam mechanics principles. Secondly, results from confined compression experiments that resemble loading of cartilage in confinement, showed nonlinear material responses for all scaffolds. Finally, the confined creep experiments were performed to calculate the hydraulic permeability of the scaffolds using soil mechanics principles. Our results show that composite scaffolds with some modifications can be a potential candidate for use of cartilage like applications. We hope such approaches help in developing novel scaffolds for tissue engineering by providing an understanding of the mechanics and can further be used to develop graded scaffolds by targeted infusion in specific regions.

Human mesenchymal stem cells cultured on silk hydrogels with variable stiffness and growth factor differentiate into mature smooth muscle cell phenotype.

Science.gov (United States)

Floren, Michael; Bonani, Walter; Dharmarajan, Anirudh; Motta, Antonella; Migliaresi, Claudio; Tan, Wei

2016-02-01

Cell-matrix and cell-biomolecule interactions play critical roles in a diversity of biological events including cell adhesion, growth, differentiation, and apoptosis. Evidence suggests that a concise crosstalk of these environmental factors may be required to direct stem cell differentiation toward matured cell type and function. However, the culmination of these complex interactions to direct stem cells into highly specific phenotypes in vitro is still widely unknown, particularly in the context of implantable biomaterials. In this study, we utilized tunable hydrogels based on a simple high pressure CO2 method and silk fibroin (SF) the structural protein of Bombyx mori silk fibers. Modification of SF protein starting water solution concentration results in hydrogels of variable stiffness while retaining key structural parameters such as matrix pore size and β-sheet crystallinity. To further resolve the complex crosstalk of chemical signals with matrix properties, we chose to investigate the role of 3D hydrogel stiffness and transforming growth factor (TGF-β1), with the aim of correlating the effects on the vascular commitment of human mesenchymal stem cells. Our data revealed the potential to upregulate matured vascular smooth muscle cell phenotype (myosin heavy chain expression) of hMSCs by employing appropriate matrix stiffness and growth factor (within 72h). Overall, our observations suggest that chemical and physical stimuli within the cellular microenvironment are tightly coupled systems involved in the fate decisions of hMSCs. The production of tunable scaffold materials that are biocompatible and further specialized to mimic tissue-specific niche environments will be of considerable value to future tissue engineering platforms. This article investigates the role of silk fibroin hydrogel stiffness and transforming growth factor (TGF-β1), with the aim of correlating the effects on the vascular commitment of human mesenchymal stem cells. Specifically, we

Silk fibroin nanostructured materials for biomedical applications

Science.gov (United States)

Mitropoulos, Alexander N.

Nanostructured biopolymers have proven to be promising to develop novel biomedical applications where forming structures at the nanoscale normally occurs by self-assembly. However, synthesizing these structures can also occur by inducing materials to transition into other forms by adding chemical cross-linkers, changing pH, or changing ionic composition. Understanding the generation of nanostructures in fluid environments, such as liquid organic solvents or supercritical fluids, has not been thoroughly examined, particularly those that are based on protein-based block-copolymers. Here, we examine the transformation of reconstituted silk fibroin, which has emerged as a promising biopolymer due to its biocompatibility, biodegradability, and ease of functionalization, into submicron spheres and gel networks which offer applications in tissue engineering and advanced sensors. Two types of gel networks, hydrogels and aerogels, have small pores and large surface areas that are defined by their structure. We design and analyze silk nanoparticle formation using a microfluidic device while offering an application for drug delivery. Additionally, we provide a model and characterize hydrogel formation from micelles to nanoparticles, while investigating cellular response to the hydrogel in an in vitro cell culture model. Lastly, we provide a second model of nanofiber formation during near-critical and supercritical drying and characterize the silk fibroin properties at different drying pressures which, when acting as a stabilizing matrix, shows to improve the activity of entrapped enzymes dried at different pressures. This work has created new nanostructured silk fibroin forms to benefit biomedical applications that could be applied to other fibrous proteins.

Facts and myths of antibacterial properties of silk.

Science.gov (United States)

Kaur, Jasjeet; Rajkhowa, Rangam; Afrin, Tarannum; Tsuzuki, Takuya; Wang, Xungai

2014-03-01

Silk cocoons provide protection to silkworm from biotic and abiotic hazards during the immobile pupal phase of the lifecycle of silkworms. Protection is particularly important for the wild silk cocoons reared in an open and harsh environment. To understand whether some of the cocoon components resist growth of microorganisms, in vitro studies were performed using gram negative bacteria Escherichia coli (E. coli) to investigate antibacterial properties of silk fiber, silk gum, and calcium oxalate crystals embedded inside some cocoons. The results show that the previously reported antibacterial properties of silk cocoons are actually due to residues of chemicals used to isolate/purify cocoon elements, and properly isolated silk fiber, gum, and embedded crystals free from such residues do not have inherent resistance to E. coli. This study removes the uncertainty created by previous studies over the presence of antibacterial properties of silk cocoons, particularly the silk gum and sericin. Copyright © 2013 Wiley Periodicals, Inc.

Drawing-induced changes in morphology and mechanical properties of hornet silk gel films.

Science.gov (United States)

Kameda, Tsunenori; Kojima, Katsura; Togawa, Eiji; Sezutsu, Hideki; Zhang, Qiang; Teramoto, Hidetoshi; Tamada, Yasushi

2010-04-12

Complete amino acid sequences of the four major proteins (Vssilk 1-4) of silk (hornet silk) obtained from yellow hornet ( Vespa simillima , Vespinae, Vespidae) cocoons have been determined. The native structure of the hornet silk (HS), in which Vssilk 1-4 have an alpha-helix domain with coiled-coil alpha-helices and a beta-sheet domain, is restored when hornet silk gel films (HSGFs) are formed by pressing and drying HS hydrogel. Necking occurs when dry HSGFs are drawn; however, wet HSGFs can be uniaxially drawn with a draw ratio (DR) of 2. Drawing helps obtain high-performance films with a maximum tensile strength and tensile modulus of 170 MPa and 5.5 GPa, respectively. Drawing-induced changes in the orientation and conformation of the coiled-coil structure are investigated.

Structure-function-property-design interplay in biopolymers: spider silk.

Science.gov (United States)

Tokareva, Olena; Jacobsen, Matthew; Buehler, Markus; Wong, Joyce; Kaplan, David L

2014-04-01

Spider silks have been a focus of research for almost two decades due to their outstanding mechanical and biophysical properties. Recent advances in genetic engineering have led to the synthesis of recombinant spider silks, thus helping to unravel a fundamental understanding of structure-function-property relationships. The relationships between molecular composition, secondary structures and mechanical properties found in different types of spider silks are described, along with a discussion of artificial spinning of these proteins and their bioapplications, including the role of silks in biomineralization and fabrication of biomaterials with controlled properties. Copyright © 2013 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Antifouling properties of hydrogels

International Nuclear Information System (INIS)

Murosaki, Takayuki; Gong, Jian Ping; Ahmed, Nafees

2011-01-01

Marine sessile organisms easily adhere to submerged solids such as rocks, metals and plastics, but not to seaweeds and fishes, which are covered with soft and wet 'hydrogel'. Inspired by this fact, we have studied long-term antifouling properties of hydrogels against marine sessile organisms. Hydrogels, especially those containing hydroxy group and sulfonic group, show excellent antifouling activity against barnacles both in laboratory assays and in the marine environment. The extreme low settlement on hydrogels in vitro and in vivo is mainly caused by antifouling properties against the barnacle cypris. (topical review)

Antifouling properties of hydrogels

Directory of Open Access Journals (Sweden)

Takayuki Murosaki, Nafees Ahmed and Jian Ping Gong

2011-01-01

Full Text Available Marine sessile organisms easily adhere to submerged solids such as rocks, metals and plastics, but not to seaweeds and fishes, which are covered with soft and wet 'hydrogel'. Inspired by this fact, we have studied long-term antifouling properties of hydrogels against marine sessile organisms. Hydrogels, especially those containing hydroxy group and sulfonic group, show excellent antifouling activity against barnacles both in laboratory assays and in the marine environment. The extreme low settlement on hydrogels in vitro and in vivo is mainly caused by antifouling properties against the barnacle cypris.

Multiscale mechanisms of nutritionally induced property variation in spider silks

Science.gov (United States)

Nobbs, Madeleine; Martens, Penny J.; Tso, I-Min; Chuang, Wei-Tsung; Chang, Chung-Kai; Sheu, Hwo-Shuenn

2018-01-01

Variability in spider major ampullate (MA) silk properties at different scales has proven difficult to determine and remains an obstacle to the development of synthetic fibers mimicking MA silk performance. A multitude of techniques may be used to measure multiscale aspects of silk properties. Here we fed five species of Araneoid spider solutions that either contained protein or were protein deprived and performed silk tensile tests, small and wide-angle X-ray scattering (SAXS/WAXS), amino acid composition analyses, and silk gene expression analyses, to resolve persistent questions about how nutrient deprivation induces variations in MA silk mechanical properties across scales. Our analyses found that the properties of each spider’s silk varied differently in response to variations in their protein intake. We found changes in the crystalline and non-crystalline nanostructures to play specific roles in inducing the property variations we found. Across treatment MaSp expression patterns differed in each of the five species. We found that in most species MaSp expression and amino acid composition variations did not conform with our predictions based on a traditional MaSp expression model. In general, changes to the silk’s alanine and proline compositions influenced the alignment of the proteins within the silk’s amorphous region, which influenced silk extensibility and toughness. Variations in structural alignment in the crystalline and non-crystalline regions influenced ultimate strength independent of genetic expression. Our study provides the deepest insights thus far into the mechanisms of how MA silk properties vary from gene expression to nanostructure formations to fiber mechanics. Such knowledge is imperative for promoting the production of synthetic silk fibers. PMID:29390013

Preparation and Characterization of a Novel Hybrid Hydrogel Composed of Bombyx mori Fibroin and Poly(N-isopropylacrylamide

Directory of Open Access Journals (Sweden)

Ting Wang

2013-01-01

Full Text Available A novel hybrid hydrogel was prepared and investigated based on silkworm silk fibroin and poly(N-isopropylacrylamide (PNIPAAm. PNIPAAm was introduced to silk fibroin, the resultant composite hydrogel was examined, and freeze-dried SF/PNIPAAm scaffold was analyzed using LB-550 dynamic light scattering particle-size analyzer, circular dichroism (CD, and scanning electron microscopy (SEM. Our results suggested that the hybrid hydrogels owned the porous sponge-like structures, and the gelation time of SF/PNIPAAm hybrids decreased with an increase in temperature and concentration of each polymer. Results of rheological analysis suggested that the rheological property of resultant SF/PNIPAAm gel depended on the concentration combinations as well as the aging time, which elapsed after mixing the two polymers. Results of CD spectra demonstrated that pH showed little influence on the secondary structure of silk fibroin, and significant changes of , , and G* as surrounding increase temperature above the lower critical solution temperature (LCST.

Web building and silk properties functionally covary among species of wolf spider.

Science.gov (United States)

Lacava, Mariángeles; Camargo, Arley; Garcia, Luis F; Benamú, Marco A; Santana, Martin; Fang, Jian; Wang, Xungai; Blamires, Sean J

2018-04-15

Although phylogenetic studies have shown covariation between the properties of spider major ampullate (MA) silk and web building, both spider webs and silks are highly plastic so we cannot be sure whether these traits functionally covary or just vary across environments that the spiders occupy. As MaSp2-like proteins provide MA silk with greater extensibility, their presence is considered necessary for spider webs to effectively capture prey. Wolf spiders (Lycosidae) are predominantly non-web building, but a select few species build webs. We accordingly collected MA silk from two web-building and six non-web-building species found in semirural ecosystems in Uruguay to test whether the presence of MaSp2-like proteins (indicated by amino acid composition, silk mechanical properties and silk nanostructures) was associated with web building across the group. The web-building and non-web-building species were from disparate subfamilies so we estimated a genetic phylogeny to perform appropriate comparisons. For all of the properties measured, we found differences between web-building and non-web-building species. A phylogenetic regression model confirmed that web building and not phylogenetic inertia influences silk properties. Our study definitively showed an ecological influence over spider silk properties. We expect that the presence of the MaSp2-like proteins and the subsequent nanostructures improves the mechanical performance of silks within the webs. Our study furthers our understanding of spider web and silk co-evolution and the ecological implications of spider silk properties. © 2018 European Society For Evolutionary Biology. Journal of Evolutionary Biology © 2018 European Society For Evolutionary Biology.

Silk constructs for delivery of muskuloskeletal therapeutics

Science.gov (United States)

Meinel, Lorenz; Kaplan, David L.

2012-01-01

Silk fibroin (SF) is a biopolymer with distinguishing features from many other bio- as well as synthetic polymers. From a biomechanical and drug delivery perspective, SF combines remarkable versatility for scaffolding (solid implants, hydrogels, threads, solutions), with advanced mechanical properties and good stabilization and controlled delivery of entrapped protein and small molecule drugs, respectively. It is this combination of mechanical and pharmaceutical features which render SF so exciting for biomedical applications. his pattern along with the versatility of this biopolymer have been translated into progress for musculoskeletal applications. We review the use and potential of silk fibroin for systemic and localized delivery of therapeutics in diseases affecting the musculoskeletal system. We also present future directions for this biopolymer as well as the necessary research and development steps for their achievement. PMID:22522139

Radiation processing of silk protein (Bilateral research cooperation OAEP and JAERI. December 1998 - December 2002)

International Nuclear Information System (INIS)

2003-01-01

Thailand's production of silk, about 1,200 ton per year, also gives about 10% of silk waste which is expected to be recycled into new material (non-textile application) and to avoid environmental pollution. For this purpose, cooperative program 'radiation processing of silk protein' was conducted between OAEP (Thailand) and JAERI. Among the results already obtained are: radiation degradation of silk protein (fibroin) with gamma rays at 160 kGy, production of fine silk milled powder (<90 microns) by electron beam irradiation at 250-1000 kGy (dry method) using electron accelerator (1 MeV, 1 mA), use of antioxidant effect of silk protein on lipid peroxidation and antibacterial activity of irradiated silk protein powder, and wound dressing hydrogel mixed with silk protein and use of antibacterial activity of cross-linked silk protein/PVA hydrogel. Other topics of interest are gamma irradiation of anionic natural polymer solution for use as latex protein scavenger and gamma radiation degradation of chitosan for use as plant growth promoter and fungicide. (S. Ohno)

Curcumin-functionalized silk materials for enhancing adipogenic differentiation of bone marrow-derived human mesenchymal stem cells

Science.gov (United States)

Li, Chunmei; Luo, Tingting; Zheng, Zhaozhu; Murphy, Amanda R.; Wang, Xiaoqin; Kaplan, David L.

2014-01-01

Curcumin, a natural phenolic compound derived from the plant Curcuma longa, was physically entrapped and stabilized in silk hydrogel films and its influence on human bone marrow-derived mesenchymal stem cells (hBMSCs) was assessed related to adipogenic differentiation. The presence of curcumin significantly reduced silk gelation time and changed the porous morphology of gel matrix, but did not change the formation of silk beta-sheet structure. Based on spectrofluorimetric analysis, curcumin likely interacted with hydrophobic residues in silk, interacting with the beta-sheet domains formed in the hydrogels. The antioxidant activity of silk film-associated curcumin remained functional over at least one month in both the dry and hydrated state. Negligible curcumin was released from silk hydrogel films over 48 hours incubation in aqueous solution. For hBMSCs cultured on silk films containing more than 0.25 mg/mL curcumin, cell proliferation was inhibited while adipogenesis was significantly promoted based on transcripts as well as oil red O staining. When hBMSCs were cultured in media containing free curcumin, both proliferation and adipogenesis of hBMSCs were inhibited when curcumin concentrations exceeded 5 μM, which is more than 1,000-times higher than the level of curcumin released from the films in aqueous solution. Thus, silk film-associated curcumin exhibited different effects on hBMSC proliferation and differentiation when compared to curcumin in solution. PMID:25132274

Water-insoluble Silk Films with Silk I Structure

Energy Technology Data Exchange (ETDEWEB)

Lu, Q.; Hu, X; Wang, X; Kluge, J; Lu, S; Cebe, P; Kaplan, D

2010-01-01

Water-insoluble regenerated silk materials are normally produced by increasing the {beta}-sheet content (silk II). In the present study water-insoluble silk films were prepared by controlling the very slow drying of Bombyx mori silk solutions, resulting in the formation of stable films with a predominant silk I instead of silk II structure. Wide angle X-ray scattering indicated that the silk films stabilized by slow drying were mainly composed of silk I rather than silk II, while water- and methanol-annealed silk films had a higher silk II content. The silk films prepared by slow drying had a globule-like structure at the core surrounded by nano-filaments. The core region was composed of silk I and silk II, surrounded by hydrophilic nano-filaments containing random turns and {alpha}-helix secondary structures. The insoluble silk films prepared by slow drying had unique thermal, mechanical and degradative properties. Differential scanning calorimetry results revealed that silk I crystals had stable thermal properties up to 250 C, without crystallization above the T{sub g}, but degraded at lower temperatures than silk II structure. Compared with water- and methanol-annealed films the films prepared by slow drying had better mechanical ductility and were more rapidly enzymatically degraded, reflecting the differences in secondary structure achieved via differences in post processing of the cast silk films. Importantly, the silk I structure, a key intermediate secondary structure for the formation of mechanically robust natural silk fibers, was successfully generated by the present approach of very slow drying, mimicking the natural process. The results also point to a new mode of generating new types of silk biomaterials with enhanced mechanical properties and increased degradation rates, while maintaining water insolubility, along with a low {beta}-sheet content.

A β-cyclodextrin, polyethyleneimine and silk fibroin hydrogel containing Centella asiatica extract and hydrocortisone acetate: releasing properties and in vivo efficacy for healing of pressure sores.

Science.gov (United States)

Lee, M S; Seo, S R; Kim, J-C

2012-10-01

  Pressure sores are lesions caused by impaired blood flow. Conventional dressings can absorb exudates, but do not promote wound healing. A hydrogel composed of β-cyclodextrin (β-CD), polyethyleneimine (PEI) and silk fibroin (SF) was assessed for use in healing of pressure sores. The hydrogel was prepared by crosslinking β-CD-grafted PEI and SF using epichlorohydrin. The gel was then immersed in an aqueous solution of Centella asiatica extract (CAE) 0.7 mg/mL and/or hydrocortisone acetate (HCA) 0.5 mg/mL. The in vivo pressure sore-healing efficacy of the dry gel (with or without the drugs) was investigated in terms of the hyperplasia of epidermis and the number of neutrophils in the skin tissue. The specific loading of CAE was 0.0091 g/g of dry gel. The percentage of CAE released at 24 h at pH 3.0, 5.0 and 7.4 was approximately 63.9%, 55.0% and 44.4%, respectively. This pH-dependent release is possibly due to the degree of gel swelling, which decreased with increasing pH. The specific loading of HCA was 0.0050 g/g dry gel, and the percentage release of HCA at 24 h was around 20% at all three pH points. It is likely that HCA release is independent of pH. HCA is a hydrophobic compound, and therefore the release of HCA is affected by the partitioning of HCA between the β-CD cavity and the bulk water phase, but not by the degree of swelling of the hydrogel. The pressure sores treated with the hydrogel healed in 6 days, compared with 10 days for controls. In this study, a β-CD/PEI/SF hydrogel containing CAE and HCA reduced the healing time for pressure sores. © The Author(s). CED © 2012 British Association of Dermatologists.

Concentration state dependence of the rheological and structural properties of reconstituted silk.

Science.gov (United States)

Mo, Chunli; Holland, Chris; Porter, David; Shao, Zhengzhong; Vollrath, Fritz

2009-10-12

The ability to control the processing of artificial silk is key to the successful application of this important and high performance biopolymer. Understanding where our current reconstitution process can be improved will not only aid us in the creation of better materials, but will also provide insight into the natural material along the way. This study aims to understand what proportion of reconstituted silk contributes to its rheological properties and what conformational state the silk proteins are in. It shows, for the first time, that a change in rheological properties can be related to a change in silk structures present in solution and reveals a low concentration gel state for silk that may have important implications for future successful artificial processing of silk.

Peptide-Graphene Interactions Enhance the Mechanical Properties of Silk Fibroin.

Science.gov (United States)

Cheng, Yuan; Koh, Leng-Duei; Li, Dechang; Ji, Baohua; Zhang, Yingyan; Yeo, Jingjie; Guan, Guijian; Han, Ming-Yong; Zhang, Yong-Wei

2015-10-07

Studies reveal that biomolecules can form intriguing molecular structures with fascinating functionalities upon interaction with graphene. Then, interesting questions arise. How does silk fibroin interact with graphene? Does such interaction lead to an enhancement in its mechanical properties? In this study, using large-scale molecular dynamics simulations, we first examine the interaction of graphene with several typical peptide structures of silk fibroin extracted from different domains of silk fibroin, including pure amorphous (P1), pure crystalline (P2), a segment from N-terminal (P3), and a combined amorphous and crystalline segment (P4), aiming to reveal their structural modifications. Our study shows that graphene can have intriguing influences on the structures formed by the peptides with sequences representing different domains of silk fibroin. In general, for protein domains with stable structure and strong intramolecular interaction (e.g., β-sheets), graphene tends to compete with the intramolecular interactions and thus weaken the interchain interaction and reduce the contents of β-sheets. For the silk domains with random or less ordered secondary structures and weak intramolecular interactions, graphene tends to enhance the stability of peptide structures; in particular, it increases the contents of helical structures. Thereafter, tensile simulations were further performed on the representative peptides to investigate how such structure modifications affect their mechanical properties. It was found that the strength and resilience of the peptides are enhanced through their interaction with graphene. The present work reveals interesting insights into the interactions between silk peptides and graphene, and contributes in the efforts to enhance the mechanical properties of silk fibroin.

Nutrient Deprivation Induces Property Variations in Spider Gluey Silk

Science.gov (United States)

Blamires, Sean J.; Sahni, Vasav; Dhinojwala, Ali; Blackledge, Todd A.; Tso, I-Min

2014-01-01

Understanding the mechanisms facilitating property variability in biological adhesives may promote biomimetic innovations. Spider gluey silks such as the spiral threads in orb webs and the gumfoot threads in cobwebs, both of which comprise of an axial thread coated by glue, are biological adhesives that have variable physical and chemical properties. Studies show that the physical and chemical properties of orb web gluey threads change when spiders are deprived of food. It is, however, unknown whether gumfoot threads undergo similar property variations when under nutritional stress. Here we tested whether protein deprivation induces similar variations in spiral and gumfoot thread morphology and stickiness. We manipulated protein intake for the orb web spider Nephila clavipes and the cobweb spider Latrodectus hesperus and measured the diameter, glue droplet volume, number of droplets per mm, axial thread width, thread stickiness and adhesive energy of their gluey silks. We found that the gluey silks of both species were stickier when the spiders were deprived of protein than when the spiders were fed protein. In N. clavipes a concomitant increase in glue droplet volume was found. Load-extension curves showed that protein deprivation induced glue property variations independent of the axial thread extensions in both species. We predicted that changes in salt composition of the glues were primarily responsible for the changes in stickiness of the silks, although changes in axial thread properties might also contribute. We, additionally, showed that N. clavipes' glue changes color under protein deprivation, probably as a consequence of changes to its biochemical composition. PMID:24523902

Comparative Study of Silk-Silk Alloy Materials

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Xue, Ye; Jao, Dave; Hu, Wenbing; Wolf, Nathan; Rocks, Eva-Marie; Hu, Xiao

Silk fibroin materials can be used for various kinds of biomedical applications. We report a comparative study of silk-silk blend materials using thermal analysis and infrared spectroscopy. Four groups of silk-silk blend films: Mori-Tussah, Mori-Muga, Mori-Eri and Mori-Thai, were fabricated from aqueous solutions and blended at different weight ratios, respectively. These silk-silk blend systems exploit the beneficial material properties of both silks. DSC and temperature-modulated DSC were used to measure the transition temperatures and heat capacity of these water-based silk-silk blend films. Fourier transform infrared spectrometer was used to characterize secondary structures of silk-silk blends. This study demonstrates that Mori silk are fully miscible with Tussah, Muga, Eri and Thai silk at different weight ratios without phase separation. Glass transition temperatures, degradation temperatures and the contents of alpha-helix and random coils of those silk-silk blend films can be controlled by changing the contents of different silks in the blend system. The features of Mori silk combined with the attributes of Tussah, Muga, Eri and Thai silk offer a useful suite of materials for a variety of applications in the future.

An Injectable Composite Gelatin Hydrogel with pH Response Properties

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Baoguo Chen

2017-01-01

Full Text Available On account of minimally invasive procedure and of filling irregular defects of tissues, injectable hydrogels are increasingly attractive in biomedical fields. However, traditional hydrogel formed by simple physical interaction or in situ crosslinking had inevitably some drawbacks such as low mechanical strength and lack of multifunctional properties. Though many investigations had successfully modified traditional injectable hydrogel to obtain both mechanical and functional properties, an acetalated β-cyclodextrin (Ac-β-CD nanoparticle composite injectable hydrogel designed in the research was another effective and efficient choice to solve the drawbacks. First of all, gelatin derivative (G-AA and Ac-β-CD were synthesized to prepare hydrogel and nanoparticle, respectively. In order to ensure good compatibility between nanoparticle and macromonomer and provide crosslink points between nanoparticle and macromonomer, G-AA was simultaneously functionalized onto the surface of Ac-β-CD nanoparticle during the fabrication of Ac-β-CD nanoparticle using one-step method. Finally, injectable composite hydrogel was obtained by photoinitiated polymerization in situ. Hydrogel properties like gelation time and swelling ratio were investigated. The viscoelastic behavior of hydrogels confirmed that typical characteristics of crosslinked elastomer for all hydrogel and nanoparticle in hydrogel could improve the mechanical property of hydrogel. Moreover, the transparency with time had verified obvious acid-response properties of hydrogels.

Silk fibroin-chondroitin sulfate scaffold with immuno-inhibition property for articular cartilage repair.

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Zhou, Feifei; Zhang, Xianzhu; Cai, Dandan; Li, Jun; Mu, Qin; Zhang, Wei; Zhu, Shouan; Jiang, Yangzi; Shen, Weiliang; Zhang, Shufang; Ouyang, Hong Wei

2017-11-01

The demand of favorable scaffolds has increased for the emerging cartilage tissue engineering. Chondroitin sulfate (CS) and silk fibroin have been investigated and reported with safety and excellent biocompatibility as tissue engineering scaffolds. However, the rapid degradation rate of pure CS scaffolds presents a challenge to effectively recreate neo-tissue similar to natural articular cartilage. Meanwhile the silk fibroin is well used as a structural constituent material because its remarkable mechanical properties, long-lasting in vivo stability and hypoimmunity. The application of composite silk fibroin and CS scaffolds for joint cartilage repair has not been well studied. Here we report that the combination of silk fibroin and CS could synergistically promote articular cartilage defect repair. The silk fibroin (silk) and silk fibroin/CS (silk-CS) scaffolds were fabricated with salt-leaching, freeze-drying and crosslinking methodologies. The biocompatibility of the scaffolds was investigated in vitro by cell adhesion, proliferation and migration with human articular chondrocytes. We found that silk-CS scaffold maintained better chondrocyte phenotype than silk scaffold; moreover, the silk-CS scaffolds reduced chondrocyte inflammatory response that was induced by interleukin (IL)-1β, which is in consistent with the well-documented anti-inflammatory activities of CS. The in vivo cartilage repair was evaluated with a rabbit osteochondral defect model. Silk-CS scaffold induced more neo-tissue formation and better structural restoration than silk scaffold after 6 and 12weeks of implantation in ICRS histological evaluations. In conclusion, we have developed a silk fibroin/ chondroitin sulfate scaffold for cartilage tissue engineering that exhibits immuno-inhibition property and can improve the self-repair capacity of cartilage. Severe cartilage defect such as osteoarthritis (OA) is difficult to self-repair because of its avascular, aneural and alymphatic nature

Design properties of hydrogel tissue-engineering scaffolds

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Zhu, Junmin; Marchant, Roger E

2011-01-01

This article summarizes the recent progress in the design and synthesis of hydrogels as tissue-engineering scaffolds. Hydrogels are attractive scaffolding materials owing to their highly swollen network structure, ability to encapsulate cells and bioactive molecules, and efficient mass transfer. Various polymers, including natural, synthetic and natural/synthetic hybrid polymers, have been used to make hydrogels via chemical or physical crosslinking. Recently, bioactive synthetic hydrogels have emerged as promising scaffolds because they can provide molecularly tailored biofunctions and adjustable mechanical properties, as well as an extracellular matrix-like microenvironment for cell growth and tissue formation. This article addresses various strategies that have been explored to design synthetic hydrogels with extracellular matrix-mimetic bioactive properties, such as cell adhesion, proteolytic degradation and growth factor-binding. PMID:22026626

Mechanical properties of silk of the Australian golden orb weavers Nephila pilipes and Nephilaplumipes.

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Kerr, Genevieve G; Nahrung, Helen F; Wiegand, Aaron; Kristoffersen, Joanna; Killen, Peter; Brown, Cameron; Macdonald, Joanne

2018-02-22

Silks from orb-weaving spiders are exceptionally tough, producing a model polymer for biomimetic fibre development. The mechanical properties of naturally spun silk threads from two species of Australian orb-weavers, Nephila pilipes and Nephila plumipes , were examined here in relation to overall thread diameter, the size and number of fibres within threads, and spider size. N. pilipes , the larger of the two species, had significantly tougher silk with higher strain capacity than its smaller congener, producing threads with average toughness of 150 MJ m -3 , despite thread diameter, mean fibre diameter and number of fibres per thread not differing significantly between the two species. Within N. pilipes , smaller silk fibres were produced by larger spiders, yielding tougher threads. In contrast, while spider size was correlated with thread diameter in N. plumipes , there were no clear patterns relating to silk toughness, which suggests that the differences in properties between the silk of the two species arise through differing molecular structure. Our results support previous studies that found that the mechanical properties of silk differ between distantly related spider species, and extends on that work to show that the mechanical and physical properties of silk from more closely related species can also differ remarkably. © 2018. Published by The Company of Biologists Ltd.

PVA hydrogel properties for biomedical application.

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Jiang, Shan; Liu, Sha; Feng, Wenhao

2011-10-01

PVA has been proposed as a promising biomaterial suitable for tissue mimicking, vascular cell culturing and vascular implanting. In this research, a kind of transparent PVA hydrogel has been investigated in order to mimic the creatural soft tissue deformation during mini-invasive surgery with needle intervention, such as brachytherapy. Three kinds of samples with the same composition of 3 g PVA, 17 g de-ionized water, 80 g dimethyl-sulfoxide but different freeze/thaw cycles have been prepared. In order to investigate the structure and properties of polyvinyl alcohol hydrogel, micro-structure, mechanical property and deformation measurement have been conducted. As the SEM image comparison results show, with the increase of freeze/thaw cycles, PVA hydrogel revealed the similar micro-structure to porcine liver tissue. With uniaxial tensile strength test, the above composition with a five freeze/thaw cycle sample resulted in Young's modulus similar to that of porcine liver's property. Through the comparison of needle insertion deformation experiment and the clinical experiment during brachytherapy, results show that the PVA hydrogel had the same deformation property as prostate tissue. These transparent hydrogel phantom materials can be suitable soft tissue substitutes in needle intervention precision or pre-operation planning studies, particularly in the cases of mimicking creatural tissue deformation and analysing video camera images. Copyright © 2011 Elsevier Ltd. All rights reserved.

Physical characterization of functionalized spider silk: electronic and sensing properties

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Eden Steven, Jin Gyu Park, Anant Paravastu, Elsa Branco Lopes, James S Brooks, Ongi Englander, Theo Siegrist, Papatya Kaner and Rufina G Alamo

2011-01-01

Full Text Available This work explores functional, fundamental and applied aspects of naturally harvested spider silk fibers. Natural silk is a protein polymer where different amino acids control the physical properties of fibroin bundles, producing, for example, combinations of β-sheet (crystalline and amorphous (helical structural regions. This complexity presents opportunities for functional modification to obtain new types of material properties. Electrical conductivity is the starting point of this investigation, where the insulating nature of neat silk under ambient conditions is described first. Modification of the conductivity by humidity, exposure to polar solvents, iodine doping, pyrolization and deposition of a thin metallic film are explored next. The conductivity increases exponentially with relative humidity and/or solvent, whereas only an incremental increase occurs after iodine doping. In contrast, iodine doping, optimal at 70 °C, has a strong effect on the morphology of silk bundles (increasing their size, on the process of pyrolization (suppressing mass loss rates and on the resulting carbonized fiber structure (that becomes more robust against bending and strain. The effects of iodine doping and other functional parameters (vacuum and thin film coating motivated an investigation with magic angle spinning nuclear magnetic resonance (MAS-NMR to monitor doping-induced changes in the amino acid-protein backbone signature. MAS-NMR revealed a moderate effect of iodine on the helical and β-sheet structures, and a lesser effect of gold sputtering. The effects of iodine doping were further probed by Fourier transform infrared (FTIR spectroscopy, revealing a partial transformation of β-sheet-to-amorphous constituency. A model is proposed, based on the findings from the MAS-NMR and FTIR, which involves iodine-induced changes in the silk fibroin bundle environment that can account for the altered physical properties. Finally, proof

Physical characterization of functionalized spider silk: electronic and sensing properties

Energy Technology Data Exchange (ETDEWEB)

Steven, Eden; Brooks, James S [Department of Physics and National High Magnetic Field Laboratory, Florida State University, 1800 East Paul Dirac, Tallahassee, FL 32310 (United States); Park, Jin Gyu [FAMU-FSU Department of Industrial and Manufacturing Engineering, High-Performance Materials Institute, Florida State University, 2005 Levy Ave., Tallahassee, FL 32310 (United States); Paravastu, Anant; Siegrist, Theo; Kaner, Papatya; Alamo, Rufina G [FAMU-FSU Department of Chemical and Biomedical Engineering and National High Magnetic Field Laboratory, Florida State University, 1800 East Paul Dirac, Tallahassee, FL 32310 (United States); Branco Lopes, Elsa [Departamento de Quimica, Instituto Tecnologico e Nuclear/CFMC-UL, P-2686-953 Sacavem (Portugal); Englander, Ongi, E-mail: esteven@magnet.fsu.edu [FAMU-FSU Department of Mechanical Engineering and National High Magnetic Field Laboratory, Florida State University, 1800 East Paul Dirac, Tallahassee, Florida 32310 (United States)

2011-10-15

This work explores functional, fundamental and applied aspects of naturally harvested spider silk fibers. Natural silk is a protein polymer where different amino acids control the physical properties of fibroin bundles, producing, for example, combinations of {beta}-sheet (crystalline) and amorphous (helical) structural regions. This complexity presents opportunities for functional modification to obtain new types of material properties. Electrical conductivity is the starting point of this investigation, where the insulating nature of neat silk under ambient conditions is described first. Modification of the conductivity by humidity, exposure to polar solvents, iodine doping, pyrolization and deposition of a thin metallic film are explored next. The conductivity increases exponentially with relative humidity and/or solvent, whereas only an incremental increase occurs after iodine doping. In contrast, iodine doping, optimal at 70 deg. C, has a strong effect on the morphology of silk bundles (increasing their size), on the process of pyrolization (suppressing mass loss rates) and on the resulting carbonized fiber structure (that becomes more robust against bending and strain). The effects of iodine doping and other functional parameters (vacuum and thin film coating) motivated an investigation with magic angle spinning nuclear magnetic resonance (MAS-NMR) to monitor doping-induced changes in the amino acid-protein backbone signature. MAS-NMR revealed a moderate effect of iodine on the helical and {beta}-sheet structures, and a lesser effect of gold sputtering. The effects of iodine doping were further probed by Fourier transform infrared (FTIR) spectroscopy, revealing a partial transformation of {beta}-sheet-to-amorphous constituency. A model is proposed, based on the findings from the MAS-NMR and FTIR, which involves iodine-induced changes in the silk fibroin bundle environment that can account for the altered physical properties. Finally, proof

Physical characterization of functionalized spider silk: electronic and sensing properties

International Nuclear Information System (INIS)

Steven, Eden; Brooks, James S; Park, Jin Gyu; Paravastu, Anant; Siegrist, Theo; Kaner, Papatya; Alamo, Rufina G; Branco Lopes, Elsa; Englander, Ongi

2011-01-01

This work explores functional, fundamental and applied aspects of naturally harvested spider silk fibers. Natural silk is a protein polymer where different amino acids control the physical properties of fibroin bundles, producing, for example, combinations of β-sheet (crystalline) and amorphous (helical) structural regions. This complexity presents opportunities for functional modification to obtain new types of material properties. Electrical conductivity is the starting point of this investigation, where the insulating nature of neat silk under ambient conditions is described first. Modification of the conductivity by humidity, exposure to polar solvents, iodine doping, pyrolization and deposition of a thin metallic film are explored next. The conductivity increases exponentially with relative humidity and/or solvent, whereas only an incremental increase occurs after iodine doping. In contrast, iodine doping, optimal at 70 deg. C, has a strong effect on the morphology of silk bundles (increasing their size), on the process of pyrolization (suppressing mass loss rates) and on the resulting carbonized fiber structure (that becomes more robust against bending and strain). The effects of iodine doping and other functional parameters (vacuum and thin film coating) motivated an investigation with magic angle spinning nuclear magnetic resonance (MAS-NMR) to monitor doping-induced changes in the amino acid-protein backbone signature. MAS-NMR revealed a moderate effect of iodine on the helical and β-sheet structures, and a lesser effect of gold sputtering. The effects of iodine doping were further probed by Fourier transform infrared (FTIR) spectroscopy, revealing a partial transformation of β-sheet-to-amorphous constituency. A model is proposed, based on the findings from the MAS-NMR and FTIR, which involves iodine-induced changes in the silk fibroin bundle environment that can account for the altered physical properties. Finally, proof-of-concept applications of

Structural and thermal properties of silk fibroin - Silver nanoparticles composite films

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Shivananda, C. S.; Rao B, B. Lakshmeesha; Shetty, G. Rajesh; Sangappa, Y.

2018-05-01

In this work, silk fibroin-silver nanoparticles (SF-AgNPs) composite films have been prepared by simple solution casting method. The composite films were examined for structural and thermal properties using X-ray diffraction (XRD), thermogravimatric (TGA) and differential scanning calorimetry (DSC) analysis. The XRD results showed that with the introduction of AgNPs in the silk fibroin matrix the amorphous nature of the silk fibroin decreases with increasing nanoparticles concentration. The silk fibroin films possess good thermal stability with the presence of AgNPs.

A Tunable Silk Hydrogel Device for Studying Limb Regeneration in Adult Xenopus Laevis.

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Anne Golding

Full Text Available In certain amphibian models limb regeneration can be promoted or inhibited by the local wound bed environment. This research introduces a device that can be utilized as an experimental tool to characterize the conditions that promotes limb regeneration in the adult frog (Xenopus laevis model. In particular, this device was designed to manipulate the local wound environment via a hydrogel insert. Initial characterization of the hydrogel insert revealed that this interaction had a significant influence on mechanical forces to the animal, due to the contraction of the hydrogel. The material and mechanical properties of the hydrogel insert were a factor in the device design in relation to the comfort of the animal and the ability to effectively manipulate the amputation site. The tunable features of the hydrogel were important in determining the pro-regenerative effects in limb regeneration, which was measured by cartilage spike formation and quantified by micro-computed tomography. The hydrogel insert was a factor in the observed morphological outcomes following amputation. Future work will focus on characterizing and optimizing the device's observed capability to manipulate biological pathways that are essential for limb regeneration. However, the present work provides a framework for the role of a hydrogel in the device and a path forward for more systematic studies.

Rationally designed synthetic protein hydrogels with predictable mechanical properties.

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Wu, Junhua; Li, Pengfei; Dong, Chenling; Jiang, Heting; Bin Xue; Gao, Xiang; Qin, Meng; Wang, Wei; Bin Chen; Cao, Yi

2018-02-12

Designing synthetic protein hydrogels with tailored mechanical properties similar to naturally occurring tissues is an eternal pursuit in tissue engineering and stem cell and cancer research. However, it remains challenging to correlate the mechanical properties of protein hydrogels with the nanomechanics of individual building blocks. Here we use single-molecule force spectroscopy, protein engineering and theoretical modeling to prove that the mechanical properties of protein hydrogels are predictable based on the mechanical hierarchy of the cross-linkers and the load-bearing modules at the molecular level. These findings provide a framework for rationally designing protein hydrogels with independently tunable elasticity, extensibility, toughness and self-healing. Using this principle, we demonstrate the engineering of self-healable muscle-mimicking hydrogels that can significantly dissipate energy through protein unfolding. We expect that this principle can be generalized for the construction of protein hydrogels with customized mechanical properties for biomedical applications.

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

Science.gov (United States)

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.

Silk Electrogel Based Gastroretentive Drug Delivery System

Science.gov (United States)

Wang, Qianrui

Gastric cancer has become a global pandemic and there is imperative to develop efficient therapies. Oral dosing strategy is the preferred route to deliver drugs for treating the disease. Recent studies suggested silk electro hydrogel, which is pH sensitive and reversible, has potential as a vehicle to deliver the drug in the stomach environment. The aim of this study is to establish in vitro electrogelation e-gel based silk gel as a gastroretentive drug delivery system. We successfully extended the duration of silk e-gel in artificial gastric juice by mixing silk solution with glycerol at different ratios before the electrogelation. Structural analysis indicated the extended duration was due to the change of beta sheet content. The glycerol mixed silk e-gel had good doxorubicin loading capability and could release doxorubicin in a sustained-release profile. Doxorubicin loaded silk e-gels were applied to human gastric cancer cells. Significant cell viability decrease was observed. We believe that with further characterization as well as functional analysis, the silk e-gel system has the potential to become an effective vehicle for gastric drug delivery applications.

Sample selection, preparation methods, and the apparent tensile properties of silkworm (B. mori) cocoon silk.

Science.gov (United States)

Reed, Emily J; Bianchini, Lindsay L; Viney, Christopher

2012-06-01

Reported literature values of the tensile properties of natural silk cover a wide range. While much of this inconsistency is the result of variability that is intrinsic to silk, some is also a consequence of differences in the way that silk is prepared for tensile tests. Here we explore how measured mechanical properties of Bombyx mori cocoon silk are affected by two intrinsic factors (the location from which the silk is collected within the cocoon, and the color of the silk), and two extrinsic factors (the storage conditions prior to testing, and different styles of reeling the fiber). We find that extrinsic and therefore controllable factors can affect the properties more than the intrinsic ones studied. Our results suggest that enhanced inter-laboratory collaborations, that lead to standardized sample collection, handling, and storage protocols prior to mechanical testing, would help to decrease unnecessary (and complicating) variation in reported tensile properties. Copyright © 2011 Wiley Periodicals, Inc.

Effects of alkyl polyglycoside (APG) on Bombyx mori silk degumming and the mechanical properties of silk fibroin fibre

Energy Technology Data Exchange (ETDEWEB)

Wang, Fei; Zhang, Yu-Qing, E-mail: sericult@suda.edu.cn

2017-05-01

Alkyl polyglycoside (APG), a nonionic surfactant, is often considered to be a green surfactant and is synthesized using glucose and long chain fatty alcohols. It is used as a degumming agent of Bombyx mori silk fibre in this study for the first time. We studied APG systematically in comparison to the traditional degumming methods, such as aqueous solutions of sodium carbonate (Na{sub 2}CO{sub 3}) and neutral soap (NS). After repeatedly boiling silk fibres in an aqueous solution of 0.25% APG three times for 30 min and using a bath ratio of 1:90–120 (g/mL), sericin was completely removed from the fibre. SDS-PAGE showed that the degumming in APG did not induce an evident breakage of the silk fibroin peptide chains, including the light chain and P25 protein. The tensile properties, thermal analysis, and scanning electron microscopic (SEM) observation of the degummed fibroin fibre all show that APG is a degumming agent similar to NS and far superior to Na{sub 2}CO{sub 3}. These results indicate that APG is an environment-friendly silk degumming/refining agent in the silk textile industry and in the manufacture of silk floss quilts. - Graphical abstract: APG has potential uses as a green degumming/refining reagent for silkworm cocoons or silk fibres in the silk industry and for sericulture production. Display Omitted.

SPIDER SILK

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PORAV Viorica

2014-05-01

Full Text Available The strengthness and toughness of spider fiber and its multifunctional nature is only surpassed in some cases by synthetic high performance fibers. In the world of natural fibers, spider silk has been long time recognized as a wonder fiber for its unique combination of high strength and rupture elongation. Scientists in civil military engineering reveal that the power of biological material (spider silk lies in the geometric configuration of structural protein, and the small cluster of week hydrogen bonds that works together to resist force and dissipate energy. Each spider and each type of silk has a set of mechanical properties optimized for their biological function. Most silks, in particular deagline silk, have exceptional mechanical properties. They exhibit a unique combination of high tensile strength and extensibility (ductility. This enables a silk fiber to absorb a lot of energy before breaking (toughness, the area under a stress- strain curve. A frequent mistake made in the mainstream media is to confuse strength and toughness when comparing silk to other materials. As shown below in detail, weight for weight, silk is stronger than steel, but not as strong as Kevlar. Silk is,however, tougher than both.This paper inform about overview on the today trend in the world of spider silk.

Structure, composition and mechanical properties of the silk fibres of ...

Indian Academy of Sciences (India)

The silk egg case and orb web of spiders are elaborate structures that are assembled from a number of components. We analysed the structure, the amino acid and fibre compositions, and the tensile properties of the silk fibres of the egg case of Nephila clavata. SEM shows that the outer and inner covers of the egg case ...

Studies on the water vapor permeability and the effect on bacterial growth of pva/sf blend hydrogels prepared by gamma irradiation for wound dressing

International Nuclear Information System (INIS)

Pongpat, Suchada; Kewsuwan, Prartana; Jetawattana, Suwimol; Piadang, Nattayana

2004-10-01

The preparation of hydrogels by gamma irradiation from poly(vinyl alcohol) (PVA) and from blend solution of PVA/silk fibroin(SF) from silk waste and some properties as wound dressing were studied. The thickness of the hydrogel was controlled to be 3 mm. Some properties of hydrogel such as water vapor permeability antibacterial activity, and protection of wound from bacteria were tested. Escherichia coli, Staphylococcus aureus, and Pseudomonas aeruginosa were used as testing cultures. The results revealed that the solution of 7% and 10% PVA and the blend solution containing 10% SF in 7% and 10% PVA (w/w) were crosslinked by γ-irradiation at the dose of 30-60 kGy. The transparent gels with good appearance were obtained. The water vapor permeability coefficients of the films were in the range of 1161.12-1527.36 g m -2 day -1 . It was found that the gels showed only an effective wound protection from the test cultures but did not show their antibacterial properties. However, remarkable reduction of bacterial growth, of about 1-2 log cycles, was also observed on the agar medium covered with the gels.p

Properties of radiation-synthesized polyvinylpyrrolidone/chitosan hydrogel blends

Energy Technology Data Exchange (ETDEWEB)

Mahmud, Maznah [School of Chemical Sciences and Food Technology, Faculty of Science and Technology, Universiti Kebangsaan Malaysia 43600 Bangi, Selangor (Malaysia); Radiation Processing Technology Division, Malaysian Nuclear Agency, 43000 Kajang, Selangor (Malaysia); Daik, Rusli [School of Chemical Sciences and Food Technology, Faculty of Science and Technology, Universiti Kebangsaan Malaysia 43600 Bangi, Selangor (Malaysia); Adam, Zainah [Radiation Processing Technology Division, Malaysian Nuclear Agency, 43000 Kajang, Selangor (Malaysia)

2015-09-25

Poly(vinylpyrrolidone) (PVP)-crosslinked chitosan hydrogels were prepared by gamma radiation at various doses; 1, 3 5, 7, 10, 15, 20, 25 and 30kGy. Gamma radiation was used as a crosslinking tool which requires no chemical initiator, no heating process and need no purification step on the end products obtained. The hydrogel formulations were composed of 6% chitosan with average molecular weight (Mw) = 48 800 g/mol and 14% PVP with Mw = 10 000 g/mol in 2% lactic acid. Physical properties of hydrogels such as gel fraction and swelling property at pH 5.5 and pH 7.0 as well as syneresis activity were determined. It was found that different radiation dose induces different effect on hydrogels’ network formed. Morphological study of hydrogels has been carried out by scanning electron microscope (SEM). From these preliminary evaluations, it can be concluded that gamma radiation is an effective tool for network development of hydrogels and it also induces enhancement on characteristics of hydrogels synthesized.

Promotion of peripheral nerve regeneration of a peptide compound hydrogel scaffold

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Wei GJ

2013-08-01

Full Text Available Guo-Jun Wei,1 Meng Yao,1 Yan-Song Wang,1 Chang-Wei Zhou,1 De-Yu Wan,1 Peng-Zhen Lei,1 Jian Wen,1 Hong-Wei Lei,2 Da-Ming Dong1 1Department of Orthopaedics, The 2nd Affiliated Hospital of Harbin Medical University, Harbin, People's Republic of China; 2Department of Rheumatology, The 2nd Affiliated Hospital of Harbin Medical University, Harbin, People's Republic of China Background: Peripheral nerve injury is a common trauma, but presents a significant challenge to the clinic. Silk-based materials have recently become an important biomaterial for tissue engineering applications due to silk’s biocompatibility and impressive mechanical and degradative properties. In the present study, a silk fibroin peptide (SF16 was designed and used as a component of the hydrogel scaffold for the repair of peripheral nerve injury. Methods: The SF16 peptide’s structure was characterized using spectrophotometry and atomic force microscopy, and the SF16 hydrogel was analyzed using scanning electron microscopy. The effects of the SF16 hydrogel on the viability and growth of live cells was first assessed in vitro, on PC12 cells. The in vivo test model involved the repair of a nerve gap with tubular nerve guides, through which it was possible to identify if the SF16 hydrogel would have the potential to enhance nerve regeneration. In this model physiological saline was set as the negative control, and collagen as the positive control. Walking track analysis and electrophysiological methods were used to evaluate the functional recovery of the nerve at 4 and 8 weeks after surgery. Results: Analysis of the SF16 peptide’s characteristics indicated that it consisted of a well-defined secondary structure and exhibited self-assembly. Results of scanning electron microscopy showed that the peptide based hydrogel may represent a porous scaffold that is viable for repair of peripheral nerve injury. Analysis of cell culture also supported that the hydrogel was an effective

Effect of polyamines on mechanical and structural properties of Bombyx mori silk.

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Yerra, Aparna; Mysarla, Danti Kumari; Siripurapu, Prasanthi; Jha, Anjali; Valluri, Satyavathi V; Mamillapalli, Anitha

2017-01-01

Silkworm, Bombyx mori (B. mori) belongs to the Lepidoptera family. The silk produced from this insect, mulberry silk, gained lot of importance as a fabric. Silk is being exploited as a biomaterial due to its surprising strength and biocompatibility. Polyamines (PA) are important cell growth regulators. In the present work the effect of treatment of polyamines, putrescine (Put), spermidine (Spd), and spermine (Spm) on the quantity and quality of silk produced was assessed. Results showed that exogenous feeding of Spd at a concentration of 50 µM increased fiber length significantly. Analysis by Fourier transform infrared (FTIR) on the properties of silk obtained from Spd treated silkworms revealed an increase in percentage of absorption with no difference in peak positions of amide I and amide III groups. Scanning electron microscopy (SEM) revealed an increase in diameter of silk. Further, analysis at molecular level showed an increase in fibroin expression in Spd treated silk glands. However, the Spd treatment showed no significant difference with respect to fibroin to sericin ratio per unit weight of cocoon, silk tenacity, and percent elongation. Thus, the present results show that polyamine treatment would influence silk quality at structural, mechanical, and molecular level in the Bombyx mori, which can be exploited in silk biomaterial production. © 2016 Wiley Periodicals, Inc.

Natural Silk as a Photonics Component: a Study on Its Light Guiding and Nonlinear Optical Properties

OpenAIRE

Kujala, Sami; Mannila, Anna; Karvonen, Lasse; Kieu, Khanh; Sun, Zhipei

2016-01-01

Silk fibers are expected to become a pathway to biocompatible and bioresorbable waveguides, which could be used to deliver localized optical power for various applications, e.g., optical therapy or imaging inside living tissue. Here, for the first time, the linear and nonlinear optical properties of natural silk fibers have been studied. The waveguiding properties of silk fibroin of largely unprocessed Bombyx mori silkworm silk are assessed using two complementary methods, and found to be on ...

Manufacturing of hydrogel biomaterials with controlled mechanical properties for tissue engineering applications.

Science.gov (United States)

Vedadghavami, Armin; Minooei, Farnaz; Mohammadi, Mohammad Hossein; Khetani, Sultan; Rezaei Kolahchi, Ahmad; Mashayekhan, Shohreh; Sanati-Nezhad, Amir

2017-10-15

Hydrogels have been recognized as crucial biomaterials in the field of tissue engineering, regenerative medicine, and drug delivery applications due to their specific characteristics. These biomaterials benefit from retaining a large amount of water, effective mass transfer, similarity to natural tissues and the ability to form different shapes. However, having relatively poor mechanical properties is a limiting factor associated with hydrogel biomaterials. Controlling the biomechanical properties of hydrogels is of paramount importance. In this work, firstly, mechanical characteristics of hydrogels and methods employed for characterizing these properties are explored. Subsequently, the most common approaches used for tuning mechanical properties of hydrogels including but are not limited to, interpenetrating polymer networks, nanocomposites, self-assembly techniques, and co-polymerization are discussed. The performance of different techniques used for tuning biomechanical properties of hydrogels is further compared. Such techniques involve lithography techniques for replication of tissues with complex mechanical profiles; microfluidic techniques applicable for generating gradients of mechanical properties in hydrogel biomaterials for engineering complex human tissues like intervertebral discs, osteochondral tissues, blood vessels and skin layers; and electrospinning techniques for synthesis of hybrid hydrogels and highly ordered fibers with tunable mechanical and biological properties. We finally discuss future perspectives and challenges for controlling biomimetic hydrogel materials possessing proper biomechanical properties. Hydrogels biomaterials are essential constituting components of engineered tissues with the applications in regenerative medicine and drug delivery. The mechanical properties of hydrogels play crucial roles in regulating the interactions between cells and extracellular matrix and directing the cells phenotype and genotype. Despite

Silk-based biomaterials.

Science.gov (United States)

Altman, Gregory H; Diaz, Frank; Jakuba, Caroline; Calabro, Tara; Horan, Rebecca L; Chen, Jingsong; Lu, Helen; Richmond, John; Kaplan, David L

2003-02-01

Silk from the silkworm, Bombyx mori, has been used as biomedical suture material for centuries. The unique mechanical properties of these fibers provided important clinical repair options for many applications. During the past 20 years, some biocompatibility problems have been reported for silkworm silk; however, contamination from residual sericin (glue-like proteins) was the likely cause. More recent studies with well-defined silkworm silk fibers and films suggest that the core silk fibroin fibers exhibit comparable biocompatibility in vitro and in vivo with other commonly used biomaterials such as polylactic acid and collagen. Furthermore, the unique mechanical properties of the silk fibers, the diversity of side chain chemistries for 'decoration' with growth and adhesion factors, and the ability to genetically tailor the protein provide additional rationale for the exploration of this family of fibrous proteins for biomaterial applications. For example, in designing scaffolds for tissue engineering these properties are particularly relevant and recent results with bone and ligament formation in vitro support the potential role for this biomaterial in future applications. To date, studies with silks to address biomaterial and matrix scaffold needs have focused on silkworm silk. With the diversity of silk-like fibrous proteins from spiders and insects, a range of native or bioengineered variants can be expected for application to a diverse set of clinical needs.

Preparation and properties of GO-PVA composite hydrogel with oriented structure

Science.gov (United States)

Liu, Huanqing; Zhang, Gongzheng; Li, Huanjun

2017-03-01

We fabricated GO-PVA composite hydrogels with oriented structure by directional freezing and repeated freeze-thawing, which owned superior mechanical property and thermostability than PVA hydrogel. Due to physical interactions such as hydrogen bonding between surface of GO and PVA chains, GO-PVA composite hydrogel possessed higher crosslinking density and smaller pore size and can resist higher temperature and stronger force from outside than PVA hydrogel. These unique properties will endow GO-PVA hydrogel with greater potential application in biomedical materials.

Mechanical properties, structure, bioadhesion, and biocompatibility of pectin hydrogels.

Science.gov (United States)

Markov, Pavel A; Krachkovsky, Nikita S; Durnev, Eugene A; Martinson, Ekaterina A; Litvinets, Sergey G; Popov, Sergey V

2017-09-01

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

Composite hydrogels of bio-inspired protein polymers : mechanical and structural characterization

NARCIS (Netherlands)

Rombouts, W.H.

2015-01-01

In this thesis we presented various combinations of custom-designed protein polymers that formed composite hydrogels. In chapter 2, composite hydrogels were prepared by mixing silk-like block copolymers (CP2SE48CP2) with collagen-like block copolymers (T9CR4T9). We found that by

Effect of Na2CO3 degumming concentration on LiBr-formic acid-silk fibroin solution properties

Directory of Open Access Journals (Sweden)

Liu Zhi

2016-01-01

Full Text Available Salt-acid system has been proved to be of high efficiency for silk fibroin dissolution. Using salt-acid system to dissolve silk, native silk fibrils can be preserved in the regenerated solution. Increasing experiments indicate that acquirement of silk fibrils in solution is strongly associated with the degumming process. In this study, the effect of sodium carbonate degumming concentration on solution properties based on lithium bromide-formic acid dissolution system was systematically investigated. Results showed that the morphology transformation of silk fibroin in solution from nanospheres to nanofibrils is determined by sodium carbonate concentration during the degumming process. Solutions containing different silk fibroin structure exhibited different rheological behaviors and different electrospinnability, leading to different electrospun nanofibre properties. The results have guiding significance for preparation and application of silk fibroin solutions.

Adsorption Properties of Lac Dyes on Wool, Silk, and Nylon

Directory of Open Access Journals (Sweden)

Bo Wei

2013-01-01

Full Text Available There has been growing interest in the dyeing of textiles with natural dyes. The research about the adsorption properties of natural dyes can help to understand their adsorption mechanism and to control their dyeing process. This study is concerned with the kinetics and isotherms of adsorption of lac dyes on wool, silk, and nylon fibers. It was found that the adsorption kinetics of lac dyes on the three fibers followed the pseudosecond-order kinetic model, and the adsorption rate of lac dyes was the fastest for silk and the slowest for wool. The activation energies for the adsorption process on wool, silk, and nylon were found to be 107.15, 87.85, and 45.31 kJ/mol, respectively. The adsorption of lac dyes on the three fibers followed the Langmuir mechanism, indicating that the electrostatic interactions between lac dyes and those fibers occurred. The saturation values for lac adsorption on the three fibers decreased in the order of wool > silk > nylon; the Langmuir affinity constant of lac adsorption on nylon was much higher than those on wool and silk.

Spider Silk Fibers Spun from Soluble Recombinant Silk Produced in Mammalian Cells

Science.gov (United States)

Lazaris, Anthoula; Arcidiacono, Steven; Huang, Yue; Zhou, Jiang-Feng; Duguay, François; Chretien, Nathalie; Welsh, Elizabeth A.; Soares, Jason W.; Karatzas, Costas N.

2002-01-01

Spider silks are protein-based ``biopolymer'' filaments or threads secreted by specialized epithelial cells as concentrated soluble precursors of highly repetitive primary sequences. Spider dragline silk is a flexible, lightweight fiber of extraordinary strength and toughness comparable to that of synthetic high-performance fibers. We sought to ``biomimic'' the process of spider silk production by expressing in mammalian cells the dragline silk genes (ADF-3/MaSpII and MaSpI) of two spider species. We produced soluble recombinant (rc)-dragline silk proteins with molecular masses of 60 to 140 kilodaltons. We demonstrated the wet spinning of silk monofilaments spun from a concentrated aqueous solution of soluble rc-spider silk protein (ADF-3; 60 kilodaltons) under modest shear and coagulation conditions. The spun fibers were water insoluble with a fine diameter (10 to 40 micrometers) and exhibited toughness and modulus values comparable to those of native dragline silks but with lower tenacity. Dope solutions with rc-silk protein concentrations >20% and postspinning draw were necessary to achieve improved mechanical properties of the spun fibers. Fiber properties correlated with finer fiber diameter and increased birefringence.

Predicting Silk Fiber Mechanical Properties through Multiscale Simulation and Protein Design.

Science.gov (United States)

Rim, Nae-Gyune; Roberts, Erin G; Ebrahimi, Davoud; Dinjaski, Nina; Jacobsen, Matthew M; Martín-Moldes, Zaira; Buehler, Markus J; Kaplan, David L; Wong, Joyce Y

2017-08-14

Silk is a promising material for biomedical applications, and much research is focused on how application-specific, mechanical properties of silk can be designed synthetically through proper amino acid sequences and processing parameters. This protocol describes an iterative process between research disciplines that combines simulation, genetic synthesis, and fiber analysis to better design silk fibers with specific mechanical properties. Computational methods are used to assess the protein polymer structure as it forms an interconnected fiber network through shearing and how this process affects fiber mechanical properties. Model outcomes are validated experimentally with the genetic design of protein polymers that match the simulation structures, fiber fabrication from these polymers, and mechanical testing of these fibers. Through iterative feedback between computation, genetic synthesis, and fiber mechanical testing, this protocol will enable a priori prediction capability of recombinant material mechanical properties via insights from the resulting molecular architecture of the fiber network based entirely on the initial protein monomer composition. This style of protocol may be applied to other fields where a research team seeks to design a biomaterial with biomedical application-specific properties. This protocol highlights when and how the three research groups (simulation, synthesis, and engineering) should be interacting to arrive at the most effective method for predictive design of their material.

Biomimetic Hybridization of Kevlar into Silk Fibroin: Nanofibrous Strategy for Improved Mechanic Properties of Flexible Composites and Filtration Membranes.

Science.gov (United States)

Lv, Lili; Han, Xiangsheng; Zong, Lu; Li, Mingjie; You, Jun; Wu, Xiaochen; Li, Chaoxu

2017-08-22

Silk, one of the strongest natural biopolymers, was hybridized with Kevlar, one of the strongest synthetic polymers, through a biomimetic nanofibrous strategy. Regenerated silk materials have outstanding properties in transparency, biocompatibility, biodegradability and sustainability, and promising applications as diverse as in pharmaceutics, electronics, photonic devices and membranes. To compete with super mechanic properties of their natural counterpart, regenerated silk materials have been hybridized with inorganic fillers such as graphene and carbon nanotubes, but frequently lose essential mechanic flexibility. Inspired by the nanofibrous strategy of natural biomaterials (e.g., silk fibers, hemp and byssal threads of mussels) for fantastic mechanic properties, Kevlar was integrated in regenerated silk materials by combining nanometric fibrillation with proper hydrothermal treatments. The resultant hybrid films showed an ultimate stress and Young's modulus two times as high as those of pure regenerated SF films. This is not only because of the reinforcing effect of Kevlar nanofibrils, but also because of the increasing content of silk β-sheets. When introducing Kevlar nanofibrils into the membranes of silk nanofibrils assembled by regenerated silk fibroin, the improved mechanic properties further enabled potential applications as pressure-driven nanofiltration membranes and flexible substrates of electronic devices.

Optimization of the silk scaffold sericin removal process for retention of silk fibroin protein structure and mechanical properties

International Nuclear Information System (INIS)

Teh, Thomas K H; Toh, Siew-Lok; Goh, James C H

2010-01-01

In the process of removing sericin (degumming) from a raw silk scaffold, the fibroin structural integrity is often challenged, leading to mechanical depreciation. This study aims to identify the factors and conditions contributing to fibroin degradation during alkaline degumming and to perform an optimization study of the parameters involved to achieve preservation of fibroin structure and properties. The methodology involves degumming knitted silk scaffolds for various durations (5-90 min) and temperatures (60-100 0 C). Mechanical agitation and use of the refreshed solution during degumming are included to investigate how these factors contribute to degumming efficiency and fibroin preservation. Characterizations of silk fibroin morphology, mechanical properties and protein components are determined by scanning electron microscopy (SEM), single fiber tensile tests and gel electrophoresis (SDS-PAGE), respectively. Sericin removal is ascertained via SEM imaging and a protein fractionation method involving SDS-PAGE. The results show that fibroin fibrillation, leading to reduced mechanical integrity, is mainly caused by prolonged degumming duration. Through a series of optimization, knitted scaffolds are observed to be optimally degummed and experience negligible mechanical and structural degradation when subjected to alkaline degumming with mechanical agitation for 30 min at 100 0 C.

Optimization of the silk scaffold sericin removal process for retention of silk fibroin protein structure and mechanical properties

Energy Technology Data Exchange (ETDEWEB)

Teh, Thomas K H; Toh, Siew-Lok; Goh, James C H, E-mail: dosgohj@nus.edu.s, E-mail: dostkh@nus.edu.s, E-mail: bietohsl@nus.edu.s [Division of Bioengineering, National University of Singapore (Singapore)

2010-06-01

In the process of removing sericin (degumming) from a raw silk scaffold, the fibroin structural integrity is often challenged, leading to mechanical depreciation. This study aims to identify the factors and conditions contributing to fibroin degradation during alkaline degumming and to perform an optimization study of the parameters involved to achieve preservation of fibroin structure and properties. The methodology involves degumming knitted silk scaffolds for various durations (5-90 min) and temperatures (60-100 {sup 0}C). Mechanical agitation and use of the refreshed solution during degumming are included to investigate how these factors contribute to degumming efficiency and fibroin preservation. Characterizations of silk fibroin morphology, mechanical properties and protein components are determined by scanning electron microscopy (SEM), single fiber tensile tests and gel electrophoresis (SDS-PAGE), respectively. Sericin removal is ascertained via SEM imaging and a protein fractionation method involving SDS-PAGE. The results show that fibroin fibrillation, leading to reduced mechanical integrity, is mainly caused by prolonged degumming duration. Through a series of optimization, knitted scaffolds are observed to be optimally degummed and experience negligible mechanical and structural degradation when subjected to alkaline degumming with mechanical agitation for 30 min at 100 {sup 0}C.

Non-invasive monitoring of in vivo hydrogel degradation and cartilage regeneration by multiparametric MR imaging

Science.gov (United States)

Chen, Zelong; Yan, Chenggong; Yan, Shina; Liu, Qin; Hou, Meirong; Xu, Yikai; Guo, Rui

2018-01-01

Numerous biodegradable hydrogels for cartilage regeneration have been widely used in the field of tissue engineering. However, to non-invasively monitor hydrogel degradation and efficiently evaluate cartilage restoration in situ is still challenging. Methods: A ultrasmall superparamagnetic iron oxide (USPIO)-labeled cellulose nanocrystal (CNC)/silk fibroin (SF)-blended hydrogel system was developed to monitor hydrogel degradation during cartilage regeneration. The physicochemical characterization and biocompatibility of the hydrogel were evaluated in vitro. The in vivo hydrogel degradation and cartilage regeneration of different implants were assessed using multiparametric magnetic resonance imaging (MRI) and further confirmed by histological analysis in a rabbit cartilage defect model for 3 months. Results: USPIO-labeled hydrogels showed sufficient MR contrast enhancement and retained stability without loss of the relaxation rate. Neither the mechanical properties of the hydrogels nor the proliferation of bone-marrow mesenchymal stem cells (BMSCs) were affected by USPIO labeling in vitro. CNC/SF hydrogels with BMSCs degraded more quickly than the acellular hydrogels as reflected by the MR relaxation rate trends in vivo. The morphology of neocartilage was noninvasively visualized by the three-dimensional water-selective cartilage MRI scan sequence, and the cartilage repair was further demonstrated by macroscopic and histological observations. Conclusion: This USPIO-labeled CNC/SF hydrogel system provides a new perspective on image-guided tissue engineering for cartilage regeneration. PMID:29464005

Improving the mechanical properties of collagen-based membranes using silk fibroin for corneal tissue engineering.

Science.gov (United States)

Long, Kai; Liu, Yang; Li, Weichang; Wang, Lin; Liu, Sa; Wang, Yingjun; Wang, Zhichong; Ren, Li

2015-03-01

Although collagen with outstanding biocompatibility has promising application in corneal tissue engineering, the mechanical properties of collagen-based scaffolds, especially suture retention strength, must be further improved to satisfy the requirements of clinical applications. This article describes a toughness reinforced collagen-based membrane using silk fibroin. The collagen-silk fibroin membranes based on collagen [silk fibroin (w/w) ratios of 100:5, 100:10, and 100:20] were prepared by using silk fibroin and cross-linking by 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide. These membranes were analyzed by scanning electron microscopy and their optical property, and NaCl and tryptophan diffusivity had been tested. The water content was found to be dependent on the content of silk fibroin, and CS10 membrane (loading 10 wt % of silk fibroin) performed the optimal mechanical properties. Also the suture experiments have proved CS10 has high suture retention strength, which can be sutured in rabbit eyes integrally. Moreover, the composite membrane proved good biocompatibility for the proliferation of human corneal epithelial cells in vitro. Lamellar keratoplasty shows that CS10 membrane promoted complete epithelialization in 35 ± 5 days, and their transparency is restored quickly in the first month. Corneal rejection reaction, neovascularization, and keratoconus are not observed. The composite films show potential for use in the field of corneal tissue engineering. © 2014 Wiley Periodicals, Inc.

Silk I and Silk II studied by fast scanning calorimetry.

Science.gov (United States)

Cebe, Peggy; Partlow, Benjamin P; Kaplan, David L; Wurm, Andreas; Zhuravlev, Evgeny; Schick, Christoph

2017-06-01

Using fast scanning calorimetry (FSC), we investigated the glass transition and crystal melting of samples of B. mori silk fibroin containing Silk I and/or Silk II crystals. Due to the very short residence times at high temperatures during such measurements, thermal decomposition of silk protein can be significantly suppressed. FSC was performed at 2000K/s using the Mettler Flash DSC1 on fibroin films with masses around 130-270ng. Films were prepared with different crystalline fractions (ranging from 0.26 to 0.50) and with different crystal structures (Silk I, Silk II, or mixed) by varying the processing conditions. These included water annealing at different temperatures, exposure to 50%MeOH in water, or autoclaving. The resulting crystal structure was examined using wide angle X-ray scattering. Degree of crystallinity was evaluated from Fourier transform infrared (FTIR) spectroscopy and from analysis of the heat capacity increment at the glass transition temperature. Silk fibroin films prepared by water annealing at 25°C were the least crystalline and had Silk I structure. FTIR and FSC studies showed that films prepared by autoclaving or 50%MeOH exposure were the most crystalline and had Silk II structure. Intermediate crystalline fraction and mixed Silk I/Silk II structures were found in films prepared by water annealing at 37°C. FSC results indicate that Silk II crystals exhibit endotherms of narrower width and have higher mean melting temperature T m (II)=351±2.6°C, compared to Silk I crystals which melt at T m (I)=292±3.8°C. Films containing mixed Silk I/Silk II structure showed two clearly separated endothermic peaks. Evidence suggests that the two types of crystals melt separately and do not thermally interconvert on the extremely short time scale (0.065s between onset and end of melting) of the FSC experiment. Silkworm silk is a naturally occurring biomaterial. The fibroin component of silk forms two types of crystals. Silk properties depend upon the

Correlation between fibroin amino acid sequence and physical silk properties.

Science.gov (United States)

Fedic, Robert; Zurovec, Michal; Sehnal, Frantisek

2003-09-12

The fiber properties of lepidopteran silk depend on the amino acid repeats that interact during H-fibroin polymerization. The aim of our research was to relate repeat composition to insect biology and fiber strength. Representative regions of the H-fibroin genes were sequenced and analyzed in three pyralid species: wax moth (Galleria mellonella), European flour moth (Ephestia kuehniella), and Indian meal moth (Plodia interpunctella). The amino acid repeats are species-specific, evidently a diversification of an ancestral region of 43 residues, and include three types of regularly dispersed motifs: modifications of GSSAASAA sequence, stretches of tripeptides GXZ where X and Z represent bulky residues, and sequences similar to PVIVIEE. No concatenations of GX dipeptide or alanine, which are typical for Bombyx silkworms and Antheraea silk moths, respectively, were found. Despite different repeat structure, the silks of G. mellonella and E. kuehniella exhibit similar tensile strength as the Bombyx and Antheraea silks. We suggest that in these latter two species, variations in the repeat length obstruct repeat alignment, but sufficiently long stretches of iterated residues get superposed to interact. In the pyralid H-fibroins, interactions of the widely separated and diverse motifs depend on the precision of repeat matching; silk is strong in G. mellonella and E. kuehniella, with 2-3 types of long homogeneous repeats, and nearly 10 times weaker in P. interpunctella, with seven types of shorter erratic repeats. The high proportion of large amino acids in the H-fibroin of pyralids has probably evolved in connection with the spinning habit of caterpillars that live in protective silk tubes and spin continuously, enlarging the tubes on one end and partly devouring the other one. The silk serves as a depot of energetically rich and essential amino acids that may be scarce in the diet.

Duplication and concerted evolution of MiSp-encoding genes underlie the material properties of minor ampullate silks of cobweb weaving spiders.

Science.gov (United States)

Vienneau-Hathaway, Jannelle M; Brassfield, Elizabeth R; Lane, Amanda Kelly; Collin, Matthew A; Correa-Garhwal, Sandra M; Clarke, Thomas H; Schwager, Evelyn E; Garb, Jessica E; Hayashi, Cheryl Y; Ayoub, Nadia A

2017-03-14

Orb-web weaving spiders and their relatives use multiple types of task-specific silks. The majority of spider silk studies have focused on the ultra-tough dragline silk synthesized in major ampullate glands, but other silk types have impressive material properties. For instance, minor ampullate silks of orb-web weaving spiders are as tough as draglines, due to their higher extensibility despite lower strength. Differences in material properties between silk types result from differences in their component proteins, particularly members of the spidroin (spider fibroin) gene family. However, the extent to which variation in material properties within a single silk type can be explained by variation in spidroin sequences is unknown. Here, we compare the minor ampullate spidroins (MiSp) of orb-weavers and cobweb weavers. Orb-web weavers use minor ampullate silk to form the auxiliary spiral of the orb-web while cobweb weavers use it to wrap prey, suggesting that selection pressures on minor ampullate spidroins (MiSp) may differ between the two groups. We report complete or nearly complete MiSp sequences from five cobweb weaving spider species and measure material properties of minor ampullate silks in a subset of these species. We also compare MiSp sequences and silk properties of our cobweb weavers to published data for orb-web weavers. We demonstrate that all our cobweb weavers possess multiple MiSp loci and that one locus is more highly expressed in at least two species. We also find that the proportion of β-spiral-forming amino acid motifs in MiSp positively correlates with minor ampullate silk extensibility across orb-web and cobweb weavers. MiSp sequences vary dramatically within and among spider species, and have likely been subject to multiple rounds of gene duplication and concerted evolution, which have contributed to the diverse material properties of minor ampullate silks. Our sequences also provide templates for recombinant silk proteins with tailored

Polymorphic regenerated silk fibers assembled through bioinspired spinning.

Science.gov (United States)

Ling, Shengjie; Qin, Zhao; Li, Chunmei; Huang, Wenwen; Kaplan, David L; Buehler, Markus J

2017-11-09

A variety of artificial spinning methods have been applied to produce regenerated silk fibers; however, how to spin regenerated silk fibers that retain the advantages of natural silks in terms of structural hierarchy and mechanical properties remains challenging. Here, we show a bioinspired approach to spin regenerated silk fibers. First, we develop a nematic silk microfibril solution, highly viscous and stable, by partially dissolving silk fibers into microfibrils. This solution maintains the hierarchical structures in natural silks and serves as spinning dope. It is then spun into regenerated silk fibers by direct extrusion in the air, offering a useful route to generate polymorphic and hierarchical regenerated silk fibers with physical properties beyond natural fiber construction. The materials maintain the structural hierarchy and mechanical properties of natural silks, including a modulus of 11 ± 4 GPa, even higher than natural spider silk. It can further be functionalized with a conductive silk/carbon nanotube coating, responsive to changes in humidity and temperature.

Silkworms transformed with chimeric silkworm/spider silk genes spin composite silk fibers with improved mechanical properties

Science.gov (United States)

The development of a spider silk manufacturing process is of great interest. piggyBac vectors were used to create transgenic silkworms encoding chimeric silkworm/spider silk proteins. The silk fibers produced by these animals were composite materials that included chimeric silkworm/spider silk prote...

Cartilage-like mechanical properties of poly (ethylene glycol)-diacrylate hydrogels.

Science.gov (United States)

Nguyen, Quynhhoa T; Hwang, Yongsung; Chen, Albert C; Varghese, Shyni; Sah, Robert L

2012-10-01

Hydrogels prepared from poly-(ethylene glycol) (PEG) have been used in a variety of studies of cartilage tissue engineering. Such hydrogels may also be useful as a tunable mechanical material for cartilage repair. Previous studies have characterized the chemical and mechanical properties of PEG-based hydrogels, as modulated by precursor molecular weight and concentration. Cartilage mechanical properties vary substantially, with maturation, with depth from the articular surface, in health and disease, and in compression and tension. We hypothesized that PEG hydrogels could mimic a broad range of the compressive and tensile mechanical properties of articular cartilage. The objective of this study was to characterize the mechanical properties of PEG hydrogels over a broad range and with reference to articular cartilage. In particular, we assessed the effects of PEG precursor molecular weight (508 Da, 3.4 kDa, 6 kDa, and 10 kDa) and concentration (10-40%) on swelling property, equilibrium confined compressive modulus (H(A0)), compressive dynamic stiffness, and hydraulic permeability (k(p0)) of PEG hydrogels in static/dynamic confined compression tests, and equilibrium tensile modulus (E(ten)) in tension tests. As molecular weight of PEG decreased and concentration increased, hydrogels exhibited a decrease in swelling ratio (31.5-2.2), an increase in H(A0) (0.01-2.46 MPa) and E(ten) (0.02-3.5 MPa), an increase in dynamic compressive stiffness (0.055-42.9 MPa), and a decrease in k(p0) (1.2 × 10(-15) to 8.5 × 10(-15) m(2)/(Pa s)). The frequency-dependence of dynamic compressive stiffness amplitude and phase, as well as the strain-dependence of permeability, were typical of the time- and strain-dependent mechanical behavior of articular cartilage. H(A0) and E(ten) were positively correlated with the final PEG concentration, accounting for swelling. These results indicate that PEG hydrogels can be prepared to mimic many of the static and dynamic mechanical

Structure and Properties of Hydrophobic Aggregation Hydrogel with Chemical Sensitive Switch

Directory of Open Access Journals (Sweden)

Jiufang Duan

2017-01-01

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

Preparation and properties of a drug sustained-release hydrogel film

International Nuclear Information System (INIS)

Yue Ling; Yang Zhanshan; Yang Shuqin; Li Qinghua

2009-01-01

A hydrogel film of drug sustained-release was prepared to accelerate wound healing. The hydrogel films containing drug or not were prepared by the freezing and thawing process. Their properties such as the physicochemical property and the drug release behavior in vitro were studied. Effect of the freezing and thawing process on antimicrobial efficacy of the gentamicin was evaluated by diffusion method. The results indicate that swelling ratio of the hydrogel films freezed for 4h is 841.21% and their gel fraction, tensile strength and elongation at break is 96.10%, 0.222 MPa and 673.50% respectively. The antimicrobial efficacy of the gentamicin has no change. The hydrogel film contained gentamicin releases the antibiotic to peak during 6 h with the cumulative drug release rate of 59.57%. The drug releases continually up to the 5th day. The drug delivery conforms to Higuchi kinetic equation, and mechanism of the drug release is matrix diffusion. The results show that the hydrogel film prepared by the freezing and thawing process display satisfactory physicochemical properties and can be used as a drug delivery system. (authors)

Structural and thermal properties of γ – irradiated Bombyx mori silk fibroin films

Energy Technology Data Exchange (ETDEWEB)

Madhukumar, R.; Asha, S.; Rao, B. Lakshmeesha; Shivananda, C. S.; Harish, K. V.; Sangappa, E-mail: syhalabhavi@yahoo.co.in [Department of Studies in Physics, Mangalore University, Mangalagangotri, Mangalore - 574199 (India); Sarojini, B. K. [Department of Studies in Chemistry, Mangalore University, Mangalagangotri, Mangalore - 574199 (India); Somashekar, R. [Department of Studies in Physics, University of Mysore, Manasagangotri, Mysore - 570006 (India)

2015-06-24

The gamma radiation-induced change in structural and thermal properties of Bombyx mori silk fibroin films were investigated and have been correlated with the applied radiation doses. Irradiation of samples were carried out in dry air at room temperature using Co-60 source, and radiation doses are in the range of 0 - 300 kGy. Structural and thermal properties of the irradiated silk films were studied using X-ray diffraction (XRD), Differential Scanning Calorimetry (DSC) and Thermogravimetric analysis (TGA) and compared with unirradiated sample. Interesting results are discussed in this report.

A comparative study of graphene-hydrogel hybrid bionanocomposites for biosensing.

Science.gov (United States)

Burrs, S L; Vanegas, D C; Rong, Y; Bhargava, M; Mechulan, N; Hendershot, P; Yamaguchi, H; Gomes, C; McLamore, E S

2015-03-07

Hydrogels have become increasingly popular as immobilization materials for cells, enzymes and proteins for biosensing applications. Enzymatic biosensors that utilize hydrogel as an encapsulant have shown improvements over other immobilization techniques such as cross linking and covalent bonding. However, to date there are no studies which directly compare multiple hydrogel-graphene nanocomposites using the same enzyme and test conditions. This study compares the performance of four different hydrogels used as protein encapsulants in a mediator-free biosensor based on graphene-nanometal-enzyme composites. Alcohol oxidase (AOx) was encapsulated in chitosan poly-N-isopropylacrylamide (PNIPAAM), silk fibroin or cellulose nanocrystals (CNC) hydrogels, and then spin coated onto a nanoplatinum-graphene modified electrode. The transduction mechanism for the biosensor was based on AOx-catalyzed oxidation of methanol to produce hydrogen peroxide. To isolate the effect(s) of stimulus response on biosensor behavior, all experiments were conducted at 25 °C and pH 7.10. Electroactive surface area (ESA), electrochemical impedance spectroscopy (EIS), sensitivity to methanol, response time, limit of detection, and shelf life were measured for each bionanocomposite. Chitosan and PNIPAAM had the highest sensitivity (0.46 ± 0.2 and 0.3 ± 0.1 μA mM(-1), respectively) and electroactive surface area (0.2 ± 0.06 and 0.2 ± 0.02 cm(2), respectively), as well as the fastest response time (4.3 ± 0.8 and 4.8 ± 1.1 s, respectively). Silk and CNC demonstrated lower sensitivity (0.09 ± 0.02 and 0.15 ± 0.03 μA mM(-1), respectively), lower electroactive surface area (0.12 ± 0.02 and 0.09 ± 0.03 cm(2), respectively), and longer response time (8.9 ± 2.1 and 6.3 ± 0.8 s, respectively). The high porosity of chitosan, PNIPAAM, and silk gels led to excellent transport, which was significantly better than CNC bionanocomposites. Electrochemical performance of CNC bionanocomposites were

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

Science.gov (United States)

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

Phase separation and mechanical properties of an elastomeric biomaterial from spider wrapping silk and elastin block copolymers.

Science.gov (United States)

Muiznieks, Lisa D; Keeley, Fred W

2016-10-01

Elastin and silk spidroins are fibrous, structural proteins with elastomeric properties of extension and recoil. While elastin is highly extensible and has excellent recovery of elastic energy, silks are particularly strong and tough. This study describes the biophysical characterization of recombinant polypeptides designed by combining spider wrapping silk and elastin-like sequences as a strategy to rationally increase the strength of elastin-based materials while maintaining extensibility. We demonstrate a thermo-responsive phase separation and spontaneous colloid-like droplet formation from silk-elastin block copolymers, and from a 34 residue disordered region of Argiope trifasciata wrapping silk alone, and measure a comprehensive suite of tensile mechanical properties from cross-linked materials. Silk-elastin materials exhibited significantly increased strength, toughness, and stiffness compared to an elastin-only material, while retaining high failure strains and low energy loss upon recoil. These data demonstrate the mechanical tunability of protein polymer biomaterials through modular, chimeric recombination, and provide structural insights into mechanical design. © 2016 Wiley Periodicals, Inc. Biopolymers 105: 693-703, 2016. © 2016 Wiley Periodicals, Inc.

Material properties that predict preservative uptake for silicone hydrogel contact lenses.

Science.gov (United States)

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.

Mechanically Robust 3D Nanostructure Chitosan-Based Hydrogels with Autonomic Self-Healing Properties.

Science.gov (United States)

Karimi, Ali Reza; Khodadadi, Azam

2016-10-12

Fabrication of hydrogels based on chitosan (CS) with superb self-healing behavior and high mechanical and electrical properties has become a challenging and fascinating topic. Most of the conventional hydrogels lack these properties at the same time. Our objectives in this research were to synthesize, characterize, and evaluate the general properties of chitosan covalently cross-linked with zinc phthalocyanine tetra-aldehyde (ZnPcTa) framework. Our hope was to access an unprecedented self-healable three-dimensional (3D) nanostructure that would harvest the superior mechanical and electrical properties associated with chitosan. The properties of cross-linker such as the structure, steric effect, and rigidity of the molecule played important roles in determining the microstructure and properties of the resulting hydrogels. The tetra-functionalized phthalocyanines favor a dynamic Schiff-base linkage with chitosan to form a 3D porous nanostructure. Based on this strategy, the self-healing ability, as demonstrated by rheological recovery and macroscopic and microscopic observations, is introduced through dynamic covalent Schiff-base linkage between NH 2 groups in CS and benzaldehyde groups at cross-linker ends. The hydrogel was characterized using FT-IR, NMR, UV/vis, and rheological measurements. In addition, cryogenic scanning electron microscopy (cryo-SEM) was employed as a technique to visualize the internal morphology of the hydrogels. Study of the surface morphology of the hydrogel showed a 3D porous nanostructure with uniform morphology. Furthermore, incorporating the conductive nanofillers, such as carbon nanotubes (CNTs), into the structure can modulate the mechanical and electrical properties of the obtained hydrogels. Interestingly, these hydrogel nanocomposites proved to have very good film-forming properties, high modulus and strength, acceptable electrical conductivity, and excellent self-healing properties at neutral pH. Such properties can be finely tuned

Injectable silk-based biomaterials for cervical tissue augmentation: an in vitro study.

Science.gov (United States)

Brown, Joseph E; Partlow, Benjamin P; Berman, Alison M; House, Michael D; Kaplan, David L

2016-01-01

Cerclage therapy is an important treatment option for preterm birth prevention. Several patient populations benefit from cerclage therapy including patients with a classic history of cervical insufficiency; patients who present with advanced cervical dilation prior to viability; and patients with a history of preterm birth and cervical shortening. Although cerclage is an effective treatment option in some patients, it can be associated with limited efficacy and procedure complications. Development of an alternative to cerclage therapy would be an important clinical development. Here we report on an injectable, silk protein-based biomaterial for cervical tissue augmentation. The rationale for the development of an injectable biomaterial is to restore the native properties of cervical tissue. While cerclage provides support to the tissue, it does not address excessive tissue softening, which is a central feature of the pathogenesis of cervical insufficiency. Silk protein-based hydrogels, which are biocompatible and naturally degrade in vivo, are suggested as a platform for restoring the native properties of cervical tissue and improving cervical function. We sought to study the properties of an injectable, silk-based biomaterial for potential use as an alternative treatment for cervical insufficiency. These biomaterials were evaluated for mechanical tunability, biocompatibility, facile injection, and in vitro degradation. Silk protein solutions were cross-linked by an enzyme catalyzed reaction to form elastic biomaterials. Biomaterials were formulated to match the native physical properties of cervical tissue during pregnancy. The cell compatibility of the materials was assessed in vitro using cervical fibroblasts, and biodegradation was evaluated using concentrated protease solution. Tissue augmentation or bulking was demonstrated using human cervical tissue from nonpregnant hysterectomy specimens. Mechanical compression tests measured the tissue stiffness as a

Experimental design of mixture applied to study PVP hydrogels properties crosslinked by ionizing radiation

Energy Technology Data Exchange (ETDEWEB)

Alcantara, Mara Tania S.; Lugao, Ademar B., E-mail: maratalcantara@uol.com.b [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil); Taqueda, Maria Elena S. [Universidade de Sao Paulo (USP), SP (Brazil). Escola Politecnica. Dept. de Engenharia Quimica

2009-07-01

Hydrogels are three dimensional hydrophilic crosslinked polymeric networks that have capacity to swell by absorbing water or biological fluids without dissolve. Hydrogels have been widely used in different application fields from agriculture, industry and in biomedicine. The properties of a hydrogel are extremely important in selecting which materials are suitable for a specific application. So mixtures can offer hydrogels with different properties to different applications. The PVP hydrogels were prepared by gamma radiation of an aqueous polymer solution and crosslinked by gamma ray, an effective and simple method for hydrogel formation that offers some advantages over the other techniques. In this work, a mixture experimental design was used to study the relationship between polymer cross-linking and swelling properties of PVP hydrogels with PEG as plasticizer and agar as gellifier. The gel fraction was measured for every mixture specified for the experiment D-optimal designs. (author)

Experimental design of mixture applied to study PVP hydrogels properties crosslinked by ionizing radiation

International Nuclear Information System (INIS)

Alcantara, Mara Tania S.; Lugao, Ademar B.; Taqueda, Maria Elena S.

2009-01-01

Hydrogels are three dimensional hydrophilic crosslinked polymeric networks that have capacity to swell by absorbing water or biological fluids without dissolve. Hydrogels have been widely used in different application fields from agriculture, industry and in biomedicine. The properties of a hydrogel are extremely important in selecting which materials are suitable for a specific application. So mixtures can offer hydrogels with different properties to different applications. The PVP hydrogels were prepared by gamma radiation of an aqueous polymer solution and crosslinked by gamma ray, an effective and simple method for hydrogel formation that offers some advantages over the other techniques. In this work, a mixture experimental design was used to study the relationship between polymer cross-linking and swelling properties of PVP hydrogels with PEG as plasticizer and agar as gellifier. The gel fraction was measured for every mixture specified for the experiment D-optimal designs. (author)

Thermal behavior and mechanical properties of physically crosslinked PVA/Gelatin hydrogels.

Science.gov (United States)

Liu, Yurong; Geever, Luke M; Kennedy, James E; Higginbotham, Clement L; Cahill, Paul A; McGuinness, Garrett B

2010-02-01

Poly (vinyl alcohol)/Gelatin hydrogels are under active investigation as potential vascular cell culture biomaterials, tissue models and vascular implants. The PVA/Gelatin hydrogels are physically crosslinked by the freeze-thaw technique, which is followed by a coagulation bath treatment. In this study, the thermal behavior of the gels was examined by differential scanning calorimetry (DSC) and dynamic mechanical thermal analysis (DMTA). Rheological measurement and uniaxial tensile tests revealed key mechanical properties. The role of polymer fraction in relation to these mechanical properties is explored. Gelatin has no significant effect on the thermal behavior of PVA, which indicates that no substantial change occurs in the PVA crystallite due to the presence of gelatin. The glass transition temperature, melting temperature, degree of crystallinity, polymer fraction, storage modulus (G') and ultimate strength of one freeze-thaw cycle (1FT) hydrogels are inferior to those of 3FT hydrogels. With coagulation, both 1FT and 3FT hydrogels shifted to a lower value of T(g), melting temperature and polymer fraction are further increased and the degree of crystallinity is depressed. The mechanical properties of 1FT, but not 3FT, were strengthened with coagulation treatment. This study gives a detailed investigation of the microstructure formation of PVA/Gelatin hydrogel in each stage of physical treatments which helps us to explain the role of physical treatments in tuning their physical properties for biomechanical applications. Copyright 2009 Elsevier Ltd. All rights reserved.

Characterization and swelling-deswelling properties of wheat straw cellulose based semi-IPNs hydrogel.

Science.gov (United States)

Liu, Jia; Li, Qian; Su, Yuan; Yue, Qinyan; Gao, Baoyu

2014-07-17

A novel wheat straw cellulose-g-poly(potassium acrylate)/polyvinyl alcohol (WSC-g-PKA/PVA) semi-interpenetrating polymer networks (semi-IPNs) hydrogel was prepared by polymerizing wheat straw and an aqueous solution of acrylic acid (AA), and further semi-interpenetrating with PVA occurred during the chemosynthesis. The swelling and deswelling properties of WSC-g-PKA/PVA semi-IPNs hydrogel and WSC-g-PKA hydrogel were studied and compared in various pH solutions, salt solutions, temperatures, particle sizes and ionic strength. The results indicated that both hydrogels had the largest swelling capacity at pH=6, and the effect of ions on the swelling of hydrogels was in the order: Na(+)>K(+)>Mg(2+)>Ca(2+). The Schott's pseudo second order model can be effectively used to evaluate swelling kinetics of hydrogels. Moreover, the semi-IPNs hydrogel had improved swelling-deswelling properties compared with that of WSC-g-PKA hydrogel. Copyright © 2014 Elsevier Ltd. All rights reserved.

Effect of gamma-rays on some technologic properties of cocoon and filament of the silk worm (Bombyx mori L.)

International Nuclear Information System (INIS)

Binkh, T.T.; Petkov, N.; Malinova, K.

1993-01-01

The effect of irradiation of silk worm eggs with 1.00, 2.00, 3.00, 4.00, 5.00, 6.00 and 7.00 Gy gamma-rays on some major technologic properties of cocoons and filament of the mulbery silk worm was studied. Single irradiation of silk worm during the phase of highest lengthening of nucleus development causes both stimulating and inhibitory effect on the technologic properties of the cocoons and the filament. The degree of stimulation or inhibition is dependent on the irradiation dose, the specificity of technologic processes and biologic characteristics of silk worm species and hybrids. Gamma-irradiation with doses 2.00 and 3.00 Gy stimulates the increase in weight of silk covering by 2.07-8.28%, raw cocoon silkness by 0.38-3.21 points and length of cocoon filament by 40-151 m. Irradiation of silk worm eggs with 2.00-4.00 Gy gamma-rays decreases by 1.4-2.3 kg (12.61-21.91%) the quantity of raw cocoons, required for production of 1 kg grege. 9 refs., 4 tabs. (author)

High-water-content mouldable polyvinyl alcohol-borax hydrogels reinforced by well-dispersed cellulose nanoparticles: dynamic rheological properties and hydrogel formation mechanism.

Science.gov (United States)

Han, Jingquan; Lei, Tingzhou; Wu, Qinglin

2014-02-15

Cellulose nanoparticle (CNP) reinforced polyvinyl alcohol-borax (PB) hydrogels were produced via a facile approach in an aqueous system. The effects of particle size, aspect ratio, crystal structure, and surface charge of CNPs on the rheological properties of the composite hydrogels were investigated. The rheological measurements confirmed the incorporation of well-dispersed CNPs to PB system significantly enhanced the viscoelasticity and stiffness of hydrogels. The obtained free-standing, high elasticity and mouldable hydrogels exhibited self-recovery under continuous step strain and thermo-reversibility under temperature sweep. With the addition of cellulose I nanofibers, a 19-fold increase in the high-frequency plateau of storage modulus was obtained compared with that of the pure PB. CNPs acted as multifunctional crosslinking agents and nanofillers to physically and chemically bridge the 3D network hydrogel. The plausible mechanism for the multi-complexation between CNPs, polyvinyl alcohol and borax was proposed to understand the relationship between the 3D network and hydrogel properties. Copyright © 2013 Elsevier Ltd. All rights reserved.

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

Energy Technology Data Exchange (ETDEWEB)

Huang, Biao; Liu, Mingxian, E-mail: liumx@jnu.edu.cn; Long, Zheru; Shen, Yan; Zhou, Changren, E-mail: tcrz9@jnu.edu.cn

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 100–250 μm 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 2.99 MPa, while the stress at 80% strain of pure SA hydrogel is only 0.8 MPa. 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. - Highlights: • Alginate/HNTs composite hydrogels were fabricated using Ca{sup 2+} cross-linking method. • The hydrogen bond interactions between HNTs and alginate are confirmed. • HNTs can significantly enhance the mechanical properties of alginate hydrogel. • HNTs can improve the cell attachment and proliferation of alginate.

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

International Nuclear Information System (INIS)

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 100–250 μm 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 2.99 MPa, while the stress at 80% strain of pure SA hydrogel is only 0.8 MPa. 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. - Highlights: • Alginate/HNTs composite hydrogels were fabricated using Ca 2+ cross-linking method. • The hydrogen bond interactions between HNTs and alginate are confirmed. • HNTs can significantly enhance the mechanical properties of alginate hydrogel. • HNTs can improve the cell attachment and proliferation of alginate.

Hybrid Silk Fibers Dry-Spun from Regenerated Silk Fibroin/Graphene Oxide Aqueous Solutions.

Science.gov (United States)

Zhang, Chao; Zhang, Yaopeng; Shao, Huili; Hu, Xuechao

2016-02-10

Regenerated silk fibroin (RSF)/graphene oxide (GO) hybrid silk fibers were dry-spun from a mixed dope of GO suspension and RSF aqueous solution. It was observed that the presence of GO greatly affect the viscosity of RSF solution. The RSF/GO hybrid fibers showed from FTIR result lower β-sheet content compared to that of pure RSF fibers. The result of synchrotron radiation wide-angle X-ray diffraction showed that the addition of GO confined the crystallization of silk fibroin (SF) leading to the decrease of crystallinity, smaller crystallite size, and new formation of interphase zones in the artificial silks. Synchrotron radiation small-angle X-ray scattering also proved that GO sheets in the hybrid silks and blended solutions were coated with a certain thickness of interphase zones due to the complex interaction between the two components. A low addition of GO, together with the mesophase zones formed between GO and RSF, enhanced the mechanical properties of hybrid fibers. The highest breaking stress of the hybrid fibers reached 435.5 ± 71.6 MPa, 23% improvement in comparison to that of degummed silk and 72% larger than that of pure RSF silk fiber. The hybrid RSF/GO materials with good biocompatibility and enhanced mechanical properties may have potential applications in tissue engineering, bioelectronic devices, or energy storage.

Transgenic Silk Moths to Produce Spider Silk

National Research Council Canada - National Science Library

Herrera, Rene J

2008-01-01

.... Other alternatives like production of the protein that yields same or similar mechanical properties of dragline silk in microorganisms or mammalian cells, in spinning fibers from concentrated protein...

Silk Fibroin Degradation Related to Rheological and Mechanical Properties.

Science.gov (United States)

Partlow, Benjamin P; Tabatabai, A Pasha; Leisk, Gary G; Cebe, Peggy; Blair, Daniel L; Kaplan, David L

2016-05-01

Regenerated silk fibroin has been proposed as a material substrate for biomedical, optical, and electronic applications. Preparation of the silk fibroin solution requires extraction (degumming) to remove contaminants, but results in the degradation of the fibroin protein. Here, a mechanism of fibroin degradation is proposed and the molecular weight and polydispersity is characterized as a function of extraction time. Rheological analysis reveals significant changes in the viscosity of samples while mechanical characterization of cast and drawn films shows increased moduli, extensibility, and strength upon drawing. Fifteen minutes extraction time results in degraded fibroin that generates the strongest films. Structural analysis by wide angle X-ray scattering (WAXS) and Fourier transform infrared spectroscopy (FTIR) indicates molecular alignment in the drawn films and shows that the drawing process converts amorphous films into the crystalline, β-sheet, secondary structure. Most interesting, by using selected extraction times, films with near-native crystallinity, alignment, and molecular weight can be achieved; yet maximal mechanical properties for the films from regenerated silk fibroin solutions are found with solutions subjected to some degree of degradation. These results suggest that the regenerated solutions and the film casting and drawing processes introduce more complexity than native spinning processes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Uncovering the structure-function relationship in spider silk

Science.gov (United States)

Yarger, Jeffery L.; Cherry, Brian R.; van der Vaart, Arjan

2018-03-01

All spiders produce protein-based biopolymer fibres that we call silk. The most studied of these silks is spider dragline silk, which is very tough and relatively abundant compared with other types of spider silks. Considerable research has been devoted to understanding the relationship between the molecular structure and mechanical properties of spider dragline silks. In this Review, we overview experimental and computational studies that have provided a wealth of detail at the molecular level on the highly conserved repetitive core and terminal regions of spider dragline silk. We also discuss the role of the nanocrystalline β-sheets and amorphous regions in determining the properties of spider silk fibres, endowing them with strength and elasticity. Additionally, we outline imaging techniques and modelling studies that elucidate the importance of the hierarchical structure of silk fibres at the molecular level. These insights into structure-function relationships can guide the reverse engineering of spider silk to enable the production of superior synthetic fibres.

Hydrogels 2.0: improved properties with nanomaterial composites for biomedical applications

International Nuclear Information System (INIS)

Memic, Adnan; Aldhahri, Musab; Alhadrami, Hani A; Hussain, M Asif; Al Nowaiser, Fozia; Al-Hazmi, Faten; Oklu, Rahmi; Khademhosseini, Ali

2016-01-01

The incorporation of nanomaterials in hydrogels (hydrated networks of crosslinked polymers) has emerged as a useful method for generating biomaterials with tailored functionality. With the available engineering approaches it is becoming much easier to fabricate nanocomposite hydrogels that display improved performance across an array of electrical, mechanical, and biological properties. In this review, we discuss the fundamental aspects of these materials as well as recent developments that have enabled their application. Specifically, we highlight synthesis and fabrication, and the choice of nanomaterials for multifunctionality as ways to overcome current material property limitations. In addition, we review the use of nanocomposite hydrogels within the framework of biomedical and pharmaceutical disciplines. (paper)

Plasticity in Major Ampullate Silk Production in Relation to Spider Phylogeny and Ecology

Science.gov (United States)

Boutry, Cecilia; Řezáč, Milan; Blackledge, Todd Alan

2011-01-01

Spider major ampullate silk is a high-performance biomaterial that has received much attention. However, most studies ignore plasticity in silk properties. A better understanding of silk plasticity could clarify the relative importance of chemical composition versus processing of silk dope for silk properties. It could also provide insight into how control of silk properties relates to spider ecology and silk uses. We compared silk plasticity (defined as variation in the properties of silk spun by a spider under different conditions) between three spider clades in relation to their anatomy and silk biochemistry. We found that silk plasticity exists in RTA clade and orbicularian spiders, two clades that differ in their silk biochemistry. Orbiculariae seem less dependent on external spinning conditions. They probably use a valve in their spinning duct to control friction forces and speed during spinning. Our results suggest that plasticity results from different processing of the silk dope in the spinning duct. Orbicularian spiders seem to display better control of silk properties, perhaps in relation to their more complex spinning duct valve. PMID:21818328

Plasticity in major ampullate silk production in relation to spider phylogeny and ecology.

Directory of Open Access Journals (Sweden)

Cecilia Boutry

Full Text Available Spider major ampullate silk is a high-performance biomaterial that has received much attention. However, most studies ignore plasticity in silk properties. A better understanding of silk plasticity could clarify the relative importance of chemical composition versus processing of silk dope for silk properties. It could also provide insight into how control of silk properties relates to spider ecology and silk uses. We compared silk plasticity (defined as variation in the properties of silk spun by a spider under different conditions between three spider clades in relation to their anatomy and silk biochemistry. We found that silk plasticity exists in RTA clade and orbicularian spiders, two clades that differ in their silk biochemistry. Orbiculariae seem less dependent on external spinning conditions. They probably use a valve in their spinning duct to control friction forces and speed during spinning. Our results suggest that plasticity results from different processing of the silk dope in the spinning duct. Orbicularian spiders seem to display better control of silk properties, perhaps in relation to their more complex spinning duct valve.

A study on synthesis and properties of Ag nanoparticles immobilized polyacrylamide hydrogel composites

International Nuclear Information System (INIS)

Saravanan, P.; Padmanabha Raju, M.; Alam, Sarfaraz

2007-01-01

Synthesis of Ag nanoparticles containing polyacrylamide (PAm) hydrogel composites was performed by free-radical cross-linking polymerization of acrylamide monomer in an aqueous medium containing Ag + ions. The Ag nanoparticle/PAm composites exhibit faint yellow colour and are found to stable under ambient conditions, without undergoing oxidation. TEM micrographs reveal the presence of nearly spherical and well-separated Ag nanoparticles with diameters in the range of 4-7 nm. UV-vis studies apparently show the characteristic surface plasmon band at ∼415 nm, for the existence of Ag nanoparticles within the hydrogel matrix. The effect of varying Ag + ion concentration within the PAm hydrogels on the amount of formation of Ag nanoparticles, as well as on the bulk properties of hydrogel nanocomposites such as equilibrium swelling, optical and electrical properties are studied. The Ag/PAm hydrogel nanocomposites have higher swelling ratio and lower electron transfer resistance than its corresponding conventional hydrogel

Silk fibroin membranes from solvent-crystallized silk fibroin/gelatin blends: Effects of blend and solvent composition

Energy Technology Data Exchange (ETDEWEB)

Gil, Eun S. [Fiber and Polymer Science Program, North Carolina State University, Raleigh, NC 27695 (United States); Frankowski, David J. [Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695 (United States); Hudson, Samuel M. [Fiber and Polymer Science Program, North Carolina State University, Raleigh, NC 27695 (United States); Spontak, Richard J. [Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695 (United States) and Department of Materials Science and Engineering, North Carolina State University, Raleigh, NC 27695 (United States)]. E-mail: Rich_Spontak@ncsu.edu

2007-04-15

Protein membranes have been prepared by mixing gelatin (G) with Bombyx mori silk fibroin (SF) and using aqueous methanol (MeOH) to induce SF crystallization. Amorphous blends of these polymers appear quasi-homogeneous, as discerned from visual observation, electron microscopy and Fourier-transform infrared (FTIR) spectroscopy. Upon subsequent exposure to aqueous MeOH, SF undergoes a conformational change from random-coil to {beta}-sheet. This transformation occurs in pure SF, as well as in each of the G/SF blends, as discerned from FTIR spectroscopy and thermal calorimetry. The influence of MeOH-induced SF crystallization on structure and property development has been measured as functions of blend and solvent composition. By preserving a support scaffold above the G helix-to-coil transition temperature, the formation of crystalline SF networks in G/SF blends can be used to stabilize G-based hydrogels or generate SF membranes for biomaterial, pharmaceutical and gas-separation purposes. The present study not only examines the properties of G/SF blends before and after SF crystallization, but also establishes the foundation for future research into thermally-responsive G/SF bioconjugates.

Optically probing torsional superelasticity in spider silks

Energy Technology Data Exchange (ETDEWEB)

Kumar, Bhupesh; Thakur, Ashish; Panda, Biswajit; Singh, Kamal P. [Department of Physical Sciences, IISER Mohali, Sector 81, Manauli, Mohali 140306 (India)

2013-11-11

We investigate torsion mechanics of various spider silks using a sensitive optical technique. We find that spider silks are torsionally superelastic in that they can reversibly withstand great torsion strains of over 10{sup 2−3} rotations per cm before failure. Among various silks from a spider, we find the failure twist-strain is greatest in the sticky capture silk followed by dragline and egg-case silk. Our in situ laser-diffraction measurements reveal that torsional strains on the silks induce a nano-scale transverse compression in its diameter that is linear and reversible. These unique torsional properties of the silks could find applications in silk-based materials and devices.

Optically probing torsional superelasticity in spider silks

International Nuclear Information System (INIS)

Kumar, Bhupesh; Thakur, Ashish; Panda, Biswajit; Singh, Kamal P.

2013-01-01

We investigate torsion mechanics of various spider silks using a sensitive optical technique. We find that spider silks are torsionally superelastic in that they can reversibly withstand great torsion strains of over 10 2−3 rotations per cm before failure. Among various silks from a spider, we find the failure twist-strain is greatest in the sticky capture silk followed by dragline and egg-case silk. Our in situ laser-diffraction measurements reveal that torsional strains on the silks induce a nano-scale transverse compression in its diameter that is linear and reversible. These unique torsional properties of the silks could find applications in silk-based materials and devices

The influence of specific binding of collagen-silk chimeras to silk biomaterials on hMSC behavior.

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An, Bo; DesRochers, Teresa M; Qin, Guokui; Xia, Xiaoxia; Thiagarajan, Geetha; Brodsky, Barbara; Kaplan, David L

2013-01-01

Collagen-like proteins in the bacteria Streptococcus pyogenes adopt a triple-helix structure with a thermal stability similar to that of animal collagens, can be expressed in high yield in Escherichia coli and can be easily modified through molecular biology techniques. However, potential applications for such recombinant collagens are limited by their lack of higher order structure to achieve the physical properties needed for most biomaterials. To overcome this problem, the S. pyogenes collagen domain was fused to a repetitive Bombyx mori silk consensus sequence, as a strategy to direct specific non-covalent binding onto solid silk materials whose superior stability, mechanical and material properties have been previously established. This approach resulted in the successful binding of these new collagen-silk chimeric proteins to silk films and porous scaffolds, and the binding affinity could be controlled by varying the number of repeats in the silk sequence. To explore the potential of collagen-silk chimera for regulating biological activity, integrin (Int) and fibronectin (Fn) binding sequences from mammalian collagens were introduced into the bacterial collagen domain. The attachment of bioactive collagen-silk chimeras to solid silk biomaterials promoted hMSC spreading and proliferation substantially in comparison to the controls. The ability to combine the biomaterial features of silk with the biological activities of collagen allowed more rapid cell interactions with silk-based biomaterials, improved regulation of stem cell growth and differentiation, as well as the formation of artificial extracellular matrices useful for tissue engineering applications. Copyright © 2012 Elsevier Ltd. All rights reserved.

Properties and toughening mechanisms of PVA/PAM double-network hydrogels prepared by freeze-thawing and anneal-swelling.

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Ou, Kangkang; Dong, Xia; Qin, Chengling; Ji, Xinan; He, Jinxin

2017-08-01

It is well known that preparation method of hydrogels has a significant effect on their properties. In this paper, freeze-thawing and anneal-swelling were applied to prepare poly(vinyl alcohol)/polyacrylamide (PVA/PAM) double-network hydrogels with covalently and physically cross-linked networks. The properties of these hydrogels were investigated and compared to control hydrogels. Results indicated that hydrogels fabricated by freeze-thawing show larger pores size and higher swelling capacity than those made by anneal-swelling and control hydrogels. Hydrogels prepared by anneal-swelling exhibit higher mechanical strength, energy dissipation, fracture energy, gel fraction and crystallinity than those made by freeze-thawing and control hydrogels. Physical cross-linking plays a key role in formation of physical-chemical double-network. The toughening mechanism of double-network hydrogel is related to their chain-fracture behavior and elasticity. The results also indicated that appropriate methods can endow hydrogels with specific microstructures and properties which would broaden current hydrogels research and applications in biomedical fields. Copyright © 2017 Elsevier B.V. All rights reserved.

Silk fibroin in tissue engineering.

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Kasoju, Naresh; Bora, Utpal

2012-07-01

Tissue engineering (TE) is a multidisciplinary field that aims at the in vitro engineering of tissues and organs by integrating science and technology of cells, materials and biochemical factors. Mimicking the natural extracellular matrix is one of the critical and challenging technological barriers, for which scaffold engineering has become a prime focus of research within the field of TE. Amongst the variety of materials tested, silk fibroin (SF) is increasingly being recognized as a promising material for scaffold fabrication. Ease of processing, excellent biocompatibility, remarkable mechanical properties and tailorable degradability of SF has been explored for fabrication of various articles such as films, porous matrices, hydrogels, nonwoven mats, etc., and has been investigated for use in various TE applications, including bone, tendon, ligament, cartilage, skin, liver, trachea, nerve, cornea, eardrum, dental, bladder, etc. The current review extensively covers the progress made in the SF-based in vitro engineering and regeneration of various human tissues and identifies opportunities for further development of this field. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Characterization of the Properties of Photopatterned Hydrogels for Use in Regenerative Medicine

Science.gov (United States)

Fiedler, Callie Irene

The goal of this thesis was to locally photopattern cytocompatible hydrogels to exhibit a wide range of mechanical properties and to probe the fundamental parameters governing these materials printed via stereolithography (SLA). Fabricating cell-laden structures with locally defined mechanical properties is non-trivial because the use of multiple precursor materials is wasteful, slow, and can lead to cell-death. To investigate the range of mechanical properties a single precursor solution can produce, I initially formed a single-network hydrogel and cyclically in- swelled fresh precursor solution followed by photo-exposure of the swollen gel ("swelling + exposure" or SE cycle). Because transport (i.e., diffusion and swelling) can occur on the same time scale as photopolymerization reaction kinetics, I first characterized the variable modulus hydrogels in bulk to isolate the reaction kinetics. In these experiments, I demonstrated the ability modify the mechanical and chemical (i.e., compressive modulus, toughness, crosslink density, swelling ratio) properties by up to 10-fold using only 2-4 SE cycles. I then used the understanding gained via these bulk experiments to locally photopattern the elastic modulus of a cytocompatible hydrogel with pixel-limited resolution (˜10s mum) employing a custom SLA system. Here I demonstrated the ability to fabricate hydrogels with a 500% elastic moduli increase with respect to the unpatterned hydrogel using atomic force microscopy. I monitored monomer attachment to the existing matrix as a function of SE cycle using confocal fluorescence microscopy to characterize the shape and size of printed features. I validated that the dependence of these features on material and processing conditions could be explained by a first-order reaction/diffusion model. With this understanding, I fabricated SLA 3D printed, soft, cytocompatible hydrogels (˜10s kPa) with ˜250 mum channels in addition to fabricating 3D printed stiff, cytocompatible

Synthesis of PVA/PVP hydrogels having two-layer by radiation and their physical properties

International Nuclear Information System (INIS)

Park, K.R.; Nho, Y.C.

2003-01-01

In these studies, two-layer hydrogels which consisted of polyurethane membrane and a mixture of polyvinyl alcohol(PVA)/poly-N-vinylpyrrolidone(PVP)/glycerin/chitosan were made for the wound dressing. Polyurethane was dissolved in solvent, the polyurethane solution was poured on the mould, and then dried to make the thin membrane. Hydrophilic polymer solutions were poured on the polyurethane membranes, they were exposed to gamma irradiation or two steps of 'freezing and thawing' and gamma irradiation doses to make the hydrogels. The physical properties such as gelation, water absorptivity, and gel strength were examined to evaluate the hydrogels for wound dressing. The physical properties of hydrogels such as gelation and gel strength was greatly improved when polyurethane membrane was used as a covering layer of hydrogel, and the evaporation speed of water in hydrogel was reduced

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

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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.

Self-assembly of cationic multidomain peptide hydrogels: supramolecular nanostructure and rheological properties dictate antimicrobial activity

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Jiang, Linhai; Xu, Dawei; Sellati, Timothy J.; Dong, He

2015-11-01

Hydrogels are an important class of biomaterials that have been widely utilized for a variety of biomedical/medical applications. The biological performance of hydrogels, particularly those used as wound dressing could be greatly advanced if imbued with inherent antimicrobial activity capable of staving off colonization of the wound site by opportunistic bacterial pathogens. Possessing such antimicrobial properties would also protect the hydrogel itself from being adversely affected by microbial attachment to its surface. We have previously demonstrated the broad-spectrum antimicrobial activity of supramolecular assemblies of cationic multi-domain peptides (MDPs) in solution. Here, we extend the 1-D soluble supramolecular assembly to 3-D hydrogels to investigate the effect of the supramolecular nanostructure and its rheological properties on the antimicrobial activity of self-assembled hydrogels. Among designed MDPs, the bactericidal activity of peptide hydrogels was found to follow an opposite trend to that in solution. Improved antimicrobial activity of self-assembled peptide hydrogels is dictated by the combined effect of supramolecular surface chemistry and storage modulus of the bulk materials, rather than the ability of individual peptides/peptide assemblies to penetrate bacterial cell membrane as observed in solution. The structure-property-activity relationship developed through this study will provide important guidelines for designing biocompatible peptide hydrogels with built-in antimicrobial activity for various biomedical applications.Hydrogels are an important class of biomaterials that have been widely utilized for a variety of biomedical/medical applications. The biological performance of hydrogels, particularly those used as wound dressing could be greatly advanced if imbued with inherent antimicrobial activity capable of staving off colonization of the wound site by opportunistic bacterial pathogens. Possessing such antimicrobial properties would

SILK FIBRE DEGRADATION AND ANALYSIS BY PROTEOMICS

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YUKSELOGLU S.Muge

2016-05-01

Full Text Available Silk is one of the promising natural fibres and has a long established history in textile production throughout the centuries. Silk is produced by cultured silk worms, spiders, scorpions, mites and flies. It is extracellular proteinaceous fibres which consist of highly crystalline and insoluble proteins, the fibroins glued with sericin and an amourphous protein. On the other hand, understanding and controlling the degradation of protein materials are important for determining quality and the value of appearance retention in textiles. Hence, for silk textiles, appearance retention is critical value for the quality. And this is one of the key properties directly related to the degree and nature of protein degradation. It is therefore necessary to understand the silk composition and damage to obtain good conservation treatments and long-term preservation especially for the historical silk fabrics. In this study, silk fibre and its properties are briefly introduced along with images on their fibre damages. Additionally, proteomics method which helps to understand the degradation at the molecular level in textiles is introduced. Finally, proteomic evaluation of silk is summarized according to the researchers carried out in the literature.

Preparation and properties of fast temperature-responsive soy protein/PNIPAAm IPN hydrogels

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Liu Yong

2014-01-01

Full Text Available The interpenetrating polymer network of fast temperature-responsive hydrogels based on soy protein and poly(N-isopropylacrylamide were successfully prepared using the sodium bicarbonate (NaHCO3 solutions as the reaction medium. The structure and properties of the hydrogels were characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, differential scanning calorimetry and thermal gravimetric analysis. The swelling and deswelling kinetics were also investigated in detail. The results have shown that the proposed hydrogels had high porous structure, good miscibility and thermal stability, and fast temperature responsivity. The presence of NaHCO3 had little effect on the volume phase transition temperature (VPTT of the hydrogels, and the VPTTs were at about 32°C. Compared with the traditional hydrogels, the proposed hydrogels had much faster swelling and deswelling rate. The swelling mechanism of the hydrogels was the non-Fickian diffusion. This fast temperature-responsive hydrogels may have potential applications in the field of biomedical materials.

Physically crosslinked composite hydrogels of PVA with natural macromolecules: structure, mechanical properties, and endothelial cell compatibility.

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Liu, Y; Vrana, N E; Cahill, P A; McGuinness, G B

2009-08-01

Polyvinyl alcohol (PVA) hydrogels have been considered potentially suitable for applications as engineered blood vessels because of their structure and mechanical properties. However, PVA's hydrophilicity hinders its capacity to act as a substrate for cell attachment. As a remedy, PVA was blended with chitosan, gelatin, or starch, and hydrogels were formed by subjecting the solutions to freeze-thaw cycles followed by coagulation bath immersion. The structure-property relationships for these hydrogels were examined by measurement of their swelling, rehydration, degradation, and mechanical properties. For the case of pure PVA hydrogels, the equilibrium swelling ratio was used to predict the effect of freeze thaw cycles and coagulation bath on average molecular weights between crosslinks and on mesh size. For all hydrogels, trends for the reswelling ratio, which is indicative of the crosslinked polymer fraction, were consistent with relative tensile properties. The coagulation bath treatment increased the degradation resistance of the hydrogels significantly. The suitability of each hydrogel for cell attachment and proliferation was examined by protein adsorption and bovine vascular endothelial cell culture experiments. Protein adsorption and cell proliferation was highest on the PVA/gelatin hydrogels. This study demonstrates that the potential of PVA hydrogels for artificial blood vessel applications can be improved by the addition of natural polymers, and that freeze-thawing and coagulation bath treatment can be utilized for fine adjustment of the physical characteristics.

Significance of Glucose Addition on Chitosan-Glycerophosphate Hydrogel Properties

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Dian Susanthy

2016-03-01

Full Text Available Chitosan-glycerophosphate hydrogel can be used as dental scaffold due to its thermosensitivity, gelation performance at body temperature, suitable acidity for body condition, biocompatibility, and ability to provide good environment for cell proliferation and differentiation. Previous study showed that glucose addition to the chitosan solution before steam sterilization improved its hydrogel mechanical strength. However, the effectiveness of glucose addition was still doubted because glucose might undergo Maillard reaction in that particular condition. The aims of this study are to confirm whether the glucose addition can increase the hydrogel mechanical strength and gelation rate effectively and also to compare their performance to be dental scaffold. This research was performed through several steps, namely preparation of chitosan-glycerophosphate solution, addition of glucose, gelation time test, gel mechanical strength measurement, functional group analysis, and physical properties measurements (pH, viscosity, and pore size. The result showed that glucose addition did not improve the hydrogel mechanical strength and gelation rate, neither when it was added before nor after steam sterilization. Glucose addition before steam sterilization seemed to trigger Maillard reaction or browning effect, while glucose addition after steam sterilization increased the amount of free water molecules in the hydrogel. Chitosan and glycerophosphate interact physically, but interaction between chitosan and glucose seems to occur chemically and followed by the formation of free water molecules. Glucose addition decreases the solution viscosity and hydrogel pore size so the hydrogel performance as dental scaffold is lowered.

Elastin Based Cell-laden Injectable Hydrogels with Tunable Gelation, Mechanical and Biodegradation Properties

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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 dynamic magnetoviscoelastic properties of biomineralized (Fe3O4) PVP-CMC hydrogel

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Ray, Ayan; Saha, Nabanita; Saha, Petr

2017-05-01

The Polyvinylpyrrolidone (PVP) and carboxymethylcellulose (CMC) based polymer matrix was used as a template for the preparation of magnetic hydrogel. This freshly prepared PVP-CMC hydrogel template was successfully mineralized by in situ synthesis of magnetic nanoparticles (Fe3O4) via chemical co-precipitation reaction using liquid diffusion method. The present study emphasizes on the rheological behavior of non-mineralized and mineralized PVP-CMC hydrogels. Scanning Electron Microscopy (SEM), transmission electron microscopy (TEM), X-ray Diffraction (XRD) pattern, Fourier transform infrared spectroscopy (FT-TR), Vibrating sample magnetometer (VSM) and dynamic magneto rheometer were used to study the morphological, physical, chemical and magnetic properties of nanoparticle (Fe3O4) filled PVP-CMC hydrogel respectively in order to monitor how Fe3O4 magnetic nanoparticles affects the mechanical properties of the hydrogel network. The storage (G') and loss (G") moduli with a complex viscosity of the system was measured using a parallel plate rheometer. Frequency and amplitude sweep with temperature variation was performed to determine the frequency and amplitude dependent magneto viscoelastic moduli for both hydrogel samples. A strong shear thinning effect was observed in both (non-mineralized and mineralized) PVP-CMC hydrogels, which confirm that Fe3O4 filled magnetic hydrogels, are pseudoplastic in nature. This Fe3O4 filled PVP-CMC hydrogel can be considered as stimuli-responsive soft matter that may be used as an actuator in medical devices.

Experimental Investigation of Mechanical and Thermal Properties of Silica Nanoparticle-Reinforced Poly(acrylamide) Nanocomposite Hydrogels.

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Zaragoza, Josergio; Babhadiashar, Nasim; 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.

Mechanical properties of biocompatible clay/P(MEO2MA-co-OEGMA) nanocomposite hydrogels.

Science.gov (United States)

Xiang, Hengxue; Xia, Mengge; Cunningham, Alexander; Chen, Wei; Sun, Bin; Zhu, Meifang

2017-08-01

The effects of crosslinking density, polymer concentration and monomer ratio on the mechanical properties (tensile and compressive properties) of biocompatible clay/P(MEO 2 MA-co-OEGMA) nanocomposite (NC) hydrogels were investigated. These novel NC hydrogels, composed of inorganic/organic networks, were prepared via in-situ free radical polymerization. The results showed that with increasing inorganic crosslinking agent, i.e. clay concentration, an increase in the tensile strength, elongation at break and compressive strength was observed. Similarly, with increasing polymer concentration, the tensile strength and compressive strength of the NC hydrogels increased while the elongation at break decreased. Increasing the molar concentration of OEGMA in the comonomer led to an increase in the tensile strength of the NC hydrogels but a reduction in the compressive strength. Moreover, clay/P(MEO 2 MA-co-OEGMA) NC hydrogels presented good biocompatibility bolstering their application as tissue engineering scaffolds. Copyright © 2017 Elsevier Ltd. All rights reserved.

Silk nanoparticles—an emerging anticancer nanomedicine

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F. Philipp Seib

2017-03-01

Full Text Available Silk is a sustainable and ecologically friendly biopolymer with a robust clinical track record in humans for load bearing applications, in part due to its excellent mechanical properties and biocompatibility. Our ability to take bottom-up and top-down approaches for the generation of silk (inspired biopolymers has been critical in supporting the evolution of silk materials and formats, including silk nanoparticles for drug delivery. Silk nanoparticles are emerging as interesting contenders for drug delivery and are well placed to advance the nanomedicine field. This review covers the use of Bombyx mori and recombinant silks as an anticancer nanomedicine, highlighting the emerging trends and developments as well as critically assessing the current opportunities and challenges by providing a context specific assessment of this multidisciplinary field.

MWCNTs/Cellulose Hydrogels Prepared from NaOH/Urea Aqueous Solution with Improved Mechanical Properties

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Yingpu Zhang

2015-01-01

Full Text Available Novel high strength composite hydrogels were designed and synthesized by introducing multiwalled carbon nanotubes (MWCNTs into cellulose/NaOH/urea aqueous solution and then cross-linked by epichlorohydrin. MWCNTs were used to modify the matrix of cellulose. The structure and morphology of the hydrogels were characterized by Fourier transform infrared (FT-IR spectroscopy, high resolution transmission electron microscopy (HR-TEM, and scanning electron microscopy (SEM. The results from swelling testing revealed that the equilibrium swelling ratio of hydrogels decreased with the increment of MWCNTs content. Thermogravimetric analysis (TGA and dynamic mechanical analysis (DMA results demonstrated that the introduction of MWCNT into cellulose hydrogel networks remarkably improved both thermal and mechanical properties of the composite hydrogels. The preparation of MWCNTs modifiedcellulose-based composites with improved mechanical properties was the first important step towards the development of advanced functional materials.

Properties and in vitro drug release of hyaluronic acid-hydroxyethyl cellulose hydrogels for transdermal delivery of isoliquiritigenin.

Science.gov (United States)

Kong, Bong Ju; Kim, Ayoung; Park, Soo Nam

2016-08-20

In the present study, the properties of hydrogel systems based on hyaluronic acid (HA)-hydroxyethyl cellulose (HEC) were investigated for effective transdermal delivery of isoliquiritigenin (ILTG). Hydrogels were synthesized by chemical cross-linking, and network structures were characterised using scanning electron microscopy (SEM) and surface area analyser. Texture properties and swelling of HA-HEC hydrogels were found to be closely linked to cross-linker concentration and swelling medium. Water in HA-HEC hydrogels was found to exist mostly in the form of free water. The viscoelasticity and the network stabilization of the hydrogels were analysed via rheological studies. The release kinetics of the hydrogel followed Fickian diffusion mechanism. In an in vitro skin penetration study, the system substantially improved the delivery of ILTG into the skin. These results indicate that the hydrogel system composed of HA and HEC has potential as a transdermal delivery system, with cross-linking density and the swelling medium influencing the properties. Copyright © 2016 Elsevier Ltd. All rights reserved.

Enhancing surface properties of breast implants by using electrospun silk fibroin.

Science.gov (United States)

Valencia-Lazcano, A A; Román-Doval, R; De La Cruz-Burelo, E; Millán-Casarrubias, E J; Rodríguez-Ortega, A

2017-08-24

In the present study, a new electrospun silk fibroin coating of silicone breast implants with improved biocompatibility and mechanical properties was obtained. Fibrous scaffolds were produced by electrospinning a solution containing silk fibroin, derived from Bombyx mori cocoons, and polyethylene oxide (PEO) to be used as a coating of breast implants. A randomly oriented structure of fibroin/PEO was electrospun on implants as assessed by SEM analysis, roughness measurements and ATR-FTIR spectroscopy. The scaffold showed 0.25 µm diameter fibres, 0.76 µm size superficial pores, arithmetic roughness of 0.632 ± 0.12 µm and texture aspect ratio of 0.893 ± 0.04. ATR-FTIR spectroscopy demonstrates the presence of PEO and fibroin in the coating. The mechanical characterisation of the implants before and after being coated with fibroin/PEO demonstrated that the fibroin/PEO scaffold contributes to the increase in the elastic modulus from 0.392 ± 0.02 to 0.560 ± 0.03 MPa and to a more elastic behaviour of the breast implants. Using the fibroin/PEO coating, human fibroblasts seeded on this matrix increased viability up to 30% compared to conventional breast implants. Electrospun silk fibroin could represent a clinically compatible, viable form to coat breast implants. Low cytotoxicity by the fibroin coating and its physico-chemical and mechanical properties may find application in improving breast implants biocompatibility. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 2017. © 2017 Wiley Periodicals, Inc.

Effects of Polysaccharides on the physical properties of Hydrogels prepared by the application of Gamma (-γ) rays

International Nuclear Information System (INIS)

Chowdhury, M. N. K.; Alam, A. K. M. M.; Bhattacharia, S. K.; Dafader, N. C.; Haque, M. E.; Akhtar, F.

2004-06-01

The effects of polysaccharides as additives on the physical properties of hydrogels prepared by the application of gamma (-γ) rays were investigated. The polysaccharides- sago, barley and rice powder were used as additives for the preparation of hydrogel from polyvinyl alcohol (PVA) having molecular weight 72,000 by applying various doses of gamma rays. The physical properties of the prepared hydrogel, such as gel fraction, degree of swelling, water absorption- and desorption rates were determined. It is found that the gel fraction of hydrogel with barley is higher than that of hydrogel with rice powder and sago. It is also found that the water absorption- and desorption rates of hydrogel with rice powder are higher than those of hydrogel with barley and sago

Effect of the sterilization method on the properties of Bombyx mori silk fibroin films

Energy Technology Data Exchange (ETDEWEB)

George, Karina A. [Queensland Eye Institute, 41 Annerley Road, South Brisbane, Queensland 4101 (Australia); Institute of Health and Biomedical Innovation, Queensland University of Technology, Kelvin Grove, Queensland 4059 (Australia); Shadforth, Audra M.A. [Queensland Eye Institute, 41 Annerley Road, South Brisbane, Queensland 4101 (Australia); Chirila, Traian V., E-mail: traian.chirila@qei.org.au [Queensland Eye Institute, 41 Annerley Road, South Brisbane, Queensland 4101 (Australia); Australian Institute of Bioengineering and Nanotechnology, University of Queensland, St Lucia, 4072 (Australia); Faculty of Health Sciences, University of Queensland, Herston, Queensland 4006 (Australia); Faculty of Science and Engineering, Queensland University of Technology, Brisbane, Queensland 4001 (Australia); Laurent, Matthieu J. [Queensland Eye Institute, 41 Annerley Road, South Brisbane, Queensland 4101 (Australia); Ecole Superieure d' Ingenieurs de Luminy (ESIL), Universite de la Mediterranee Aix-Marseille II, Luminy case 925 13288, Marseille, Cedex 09 (France); Stephenson, Sally-Anne [Institute of Health and Biomedical Innovation, Queensland University of Technology, Kelvin Grove, Queensland 4059 (Australia); Faculty of Health, Queensland University of Technology, Brisbane, Queensland 4001 (Australia); Edwards, Grant A. [Australian Institute of Bioengineering and Nanotechnology, University of Queensland, St Lucia, 4072 (Australia); Madden, Peter W. [Queensland Eye Institute, 41 Annerley Road, South Brisbane, Queensland 4101 (Australia); Faculty of Health Sciences, University of Queensland, Herston, Queensland 4006 (Australia); and others

2013-03-01

We have compared the effects of different sterilization techniques on the properties of Bombyx mori silk fibroin thin films with the view to subsequent use for corneal tissue engineering. The transparency, tensile properties, corneal epithelial cell attachment and degradation of the films were used to evaluate the suitability of certain sterilization techniques including gamma-irradiation (in air or nitrogen), steam treatment and immersion in aqueous ethanol. The investigations showed that gamma-irradiation, performed either in air or in a nitrogen atmosphere, did not significantly alter the properties of films. The films sterilized by gamma-irradiation or by immersion in ethanol had a transparency greater than 98% and tensile properties comparable to human cornea and amniotic membrane, the materials of choice in the reconstruction of ocular surface. Although steam-sterilization produced stronger, stiffer films, they were less transparent, and cell attachment was affected by the variable topography of these films. It was concluded that gamma-irradiation should be considered to be the most suitable method for the sterilization of silk fibroin films, however, the treatment with ethanol is also an acceptable method. - Highlights: Black-Right-Pointing-Pointer The effects of four methods of sterilization on the properties of silk fibroin films were investigated. Black-Right-Pointing-Pointer Steam treatment leads to stiffer films but to lower transparency and variable surface topography. Black-Right-Pointing-Pointer Degradation of fibroin is enhanced in the films that were gamma-irradiated. Black-Right-Pointing-Pointer The effects on mechanical properties are explained through changes in both primary and secondary structure of fibroin. Black-Right-Pointing-Pointer Gamma-irradiation and immersion in aqueous ethanol are suggested as preferred methods of sterilization.

Effect of the sterilization method on the properties of Bombyx mori silk fibroin films

International Nuclear Information System (INIS)

George, Karina A.; Shadforth, Audra M.A.; Chirila, Traian V.; Laurent, Matthieu J.; Stephenson, Sally-Anne; Edwards, Grant A.; Madden, Peter W.

2013-01-01

We have compared the effects of different sterilization techniques on the properties of Bombyx mori silk fibroin thin films with the view to subsequent use for corneal tissue engineering. The transparency, tensile properties, corneal epithelial cell attachment and degradation of the films were used to evaluate the suitability of certain sterilization techniques including gamma-irradiation (in air or nitrogen), steam treatment and immersion in aqueous ethanol. The investigations showed that gamma-irradiation, performed either in air or in a nitrogen atmosphere, did not significantly alter the properties of films. The films sterilized by gamma-irradiation or by immersion in ethanol had a transparency greater than 98% and tensile properties comparable to human cornea and amniotic membrane, the materials of choice in the reconstruction of ocular surface. Although steam-sterilization produced stronger, stiffer films, they were less transparent, and cell attachment was affected by the variable topography of these films. It was concluded that gamma-irradiation should be considered to be the most suitable method for the sterilization of silk fibroin films, however, the treatment with ethanol is also an acceptable method. - Highlights: ► The effects of four methods of sterilization on the properties of silk fibroin films were investigated. ► Steam treatment leads to stiffer films but to lower transparency and variable surface topography. ► Degradation of fibroin is enhanced in the films that were gamma-irradiated. ► The effects on mechanical properties are explained through changes in both primary and secondary structure of fibroin. ► Gamma-irradiation and immersion in aqueous ethanol are suggested as preferred methods of sterilization.

Development of hybrid cotton/hydrogel yarns with improved absorption properties for biomedical applications

Energy Technology Data Exchange (ETDEWEB)

Pollini, Mauro; Paladini, Federica, E-mail: federica.paladini@unisalento.it; Sannino, Alessandro; Maffezzoli, Alfonso

2016-06-01

Hyperhidrosis, or excessive sweating, is an overlooked and potentially disabling symptom, which is often seen in social anxiety disorder. In this work an innovative advanced textile material was developed for application in the management of excessive sweating, preparing a drying yarn providing improved comfort. Hybrid cotton/hydrogel yarns were obtained by combining cotton with superabsorbent hydrogels through an optimization study focused on the achievement of the most promising product in terms of absorption properties and resistance to washings. Swelling and washing tests were performed using different hydrogels, and the effect of an additional crosslinking on the materials was also evaluated by testing different solutions containing Al{sup 3+} and Ca{sup 2+} ions. Scanning electron microscopy and infrared spectroscopy analyses were adopted to characterize morphology and chemical structure of the hydrogels undergoing different production processes. The biocompatibility of the hybrid fabrics was demonstrated by 3-[4,5-dimethylthiazol-2-yl]-2,5-diphenyltetrazolium bromide colorimetric assay (MTT) through the extract method. - Highlights: • Novel textile based on natural fibres and superabsorbent hydrogels was developed. • The swelling ratio and the durability to washings were evaluated. • The effect of the choice of the hydrogel was studied. • The effects of additional crosslinking on hydrogel and fabrics were evaluated. • The optimized parameters determined durable and improved absorption properties.

Studies on the properties of poly (ethylene oxide) R-150 hydrogel films formed by irradiation graft

International Nuclear Information System (INIS)

Yang Zhanshan; Zhu Nankang; Yang Shuqin; Qiang Yizhong

1999-01-01

In order to improve the mechanical properties of poly (ethylene oxide) (PEO) hydrogel film was used as wound dressing. The chemical and physical properties of the PEO R-150 graft hydrogel film formed by blends of electron beam irradiated-PEO R-150 and poly(vinyl alcohol) (PVA) were studied. The experimental results showed that the crosslinking densities of the PEO R-150 graft hydrogel increased along with the increasing of the irradiation doses and decreased with the increasing of the blend concentrations. While the PVA graft proportions did not produce obvious effects on the crosslinking density of the graft hydrogel. The crosslinking density of the graft hydrogel were obviously lower than that of the pure PVA hydrogel. The equilibrium water content of the graft hydrogel decrease as the irradiation dose and the PVA graft proportion increased; but they increased as the blend concentration increased. The equilibrium water content of the graft hydrogel was obviously higher than those of the pure PVA hydrogel. The hardness of the PVA hydrogel film increased with the irradiation dose. The hardness of the graft hydrogel decreased with the blend concentration, whereas it increased with the PVA graft proportion. The results suggest the PVA produces a main effect on the crosslinking density of the graft hydrogel, the PEO R-150 produces a main effect on the equilibrium water content of the graft hydrogel, and the both polymers have double effects on the hardness of the graft hydrogel

Silk: a potential medium for tissue engineering.

Science.gov (United States)

Sobajo, Cassandra; Behzad, Farhad; Yuan, Xue-Feng; Bayat, Ardeshir

2008-01-01

Human skin is a complex bilayered organ that serves as a protective barrier against the environment. The loss of integrity of skin by traumatic experiences such as burns and ulcers may result in considerable disability or ultimately death. Therefore, in skin injuries, adequate dermal substitutes are among primary care targets, aimed at replacing the structural and functional properties of native skin. To date, there are very few single application tissue-engineered dermal constructs fulfilling this criterion. Silk produced by the domestic silkworm, Bombyx mori, has a long history of use in medicine. It has recently been increasingly investigated as a promising biomaterial for dermal constructs. Silk contains 2 fibrous proteins, sericin and fibroin. Each one exhibits unique mechanical and biological properties. Comprehensive review of randomized-controlled trials investigating current dermal constructs and the structures and properties of silk-based constructs on wound healing. This review revealed that silk-fibroin is regarded as the most promising biomaterial, providing options for the construction of tissue-engineered skin. The research available indicates that silk fibroin is a suitable biomaterial scaffold for the provision of adequate dermal constructs.

DNA Hydrogel with Tunable pH-Responsive Properties Produced by Rolling Circle Amplification.

Science.gov (United States)

Xu, Wanlin; Huang, Yishun; Zhao, Haoran; Li, Pan; Liu, Guoyuan; Li, Jing; Zhu, Chengshen; Tian, Leilei

2017-12-22

Recently, smart DNA hydrogels, which are generally formed by the self-assembly of oligonucleotides or through the cross-linking of oligonucleotide-polymer hybrids, have attracted tremendous attention. However, the difficulties of fabricating DNA hydrogels limit their practical applications. We report herein a novel method for producing pH-responsive hydrogels by rolling circle amplification (RCA). In this method, pH-sensitive cross-linking sites were introduced into the polymeric DNA chains during DNA synthesis. As the DNA sequence can be precisely defined by its template, the properties of such hydrogels can be finely tuned in a very facile way through template design. We have investigated the process of hydrogel formation and pH-responsiveness to provide rationales for functional hydrogel design based on the RCA reaction. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Manufacture and Drug Delivery Applications of Silk Nanoparticles.

Science.gov (United States)

Wongpinyochit, Thidarat; Johnston, Blair F; Seib, F Philipp

2016-10-08

Silk is a promising biopolymer for biomedical and pharmaceutical applications due to its outstanding mechanical properties, biocompatibility and biodegradability, as well its ability to protect and subsequently release its payload in response to a trigger. While silk can be formulated into various material formats, silk nanoparticles are emerging as promising drug delivery systems. Therefore, this article covers the procedures for reverse engineering silk cocoons to yield a regenerated silk solution that can be used to generate stable silk nanoparticles. These nanoparticles are subsequently characterized, drug loaded and explored as a potential anticancer drug delivery system. Briefly, silk cocoons are reverse engineered first by degumming the cocoons, followed by silk dissolution and clean up, to yield an aqueous silk solution. Next, the regenerated silk solution is subjected to nanoprecipitation to yield silk nanoparticles - a simple but powerful method that generates uniform nanoparticles. The silk nanoparticles are characterized according to their size, zeta potential, morphology and stability in aqueous media, as well as their ability to entrap a chemotherapeutic payload and kill human breast cancer cells. Overall, the described methodology yields uniform silk nanoparticles that can be readily explored for a myriad of applications, including their use as a potential nanomedicine.

Dissolution and regeneration of non-mulberry Eriogyna Pyretorum silk fibroin

Science.gov (United States)

Guo, Yuhang; Li, Xiufang; Zhang, Qiang; Yan, Shuqin; You, Renchuan

2017-10-01

Protein-based materials have been actively pursued as biomaterials because of their nontoxicity, biocompatibility and biodegradability. In this work, we demonstrated the potential of Eriogyna pyretorum silk fibroin (ESF), a non-mulberry silk protein, as biomaterials. The degummed ESF fibers could be dissolved completely by Ca(NO3)2/H2O/C2H5OH solution to produce regenerated ESF. The solubility was strongly dependent on the addition of C2H5OH, heating temperature and dissolving time. α-helix and random coil are main molecular conformation in aqueous ESF solution. The sol-gel transition behavior of regenerated ESF was also studied, indicating that the conformational transition of regenerated ESF from random coil/α-helix to β-sheet during gelation. Especially, ESF showed more rapid gelation than mulberry silk fibroin (BSF). Consequently, the gelation rate of BSF could be controlled ranging from tens of minutes to days by changing the ESF ratio, providing useful options for the fabrication of silk hydrogels. Water-stable regenerated ESF film could be achieved by using aqueous ethanol to induce structural transition. Tensile tests showed that the ESF films have a dry strength of approximate 31.0 MPa and a wet strength of approximate 3.3 MPa. This study provides new opportunities as an alternative natural protein material for biomedical applications.

A Novel Domperidone Hydrogel: Preparation, Characterization, Pharmacokinetic, and Pharmacodynamic Properties

Directory of Open Access Journals (Sweden)

Chun-Hui Zhang

2011-01-01

Full Text Available The purpose of the present study was to prepare a novel domperidone hydrogel. The domperidone dispersion was prepared by the solvent evaporation method. The characteristics of domperidone dispersion were measured by dynamic light scattering (DLS, scanning electronic microscopy (SEM, differential scanning calorimetry (DSC, X-ray diffractometry, and solubility test, respectively. Domperidone hydrogel was prepared by directly incorporating the domperidone dispersion in Carbopol hydrogel to increase its mucoadhesive properties to gastrointestinal tract (GIT. The in vivo pharmacokinetic and pharmacodynamic studies were investigated to evaluate the relative oral bioavailability and the propulsion efficacy of domperidone hydrogel as compared with market domperidone tablet (Motilium tablet. The particle size of domperidone dispersion in distilled water was 454.0 nm. The results of DSC and X-ray indicated that domperidone in dispersion was in amorphous state. The solubility of domperidone in the dispersion in distilled water, pH of 1, 5, and 7 buffer solution was 45.7-, 63.9-, 13.1-, and 3.7-fold higher than that of raw domperidone, respectively. The area under the plasma concentration curve (AUC0–24 in domperidone hydrogel was 2.2-fold higher than that of tablet. The prolonged propulsion efficacy in the domperidone hydrogel group compared to that in tablet group was observed in the pharmacodynamic test.

Drying and storage effects on poly(ethylene glycol) hydrogel mechanical properties and bioactivity.

Science.gov (United States)

Luong, P T; Browning, M B; Bixler, R S; Cosgriff-Hernandez, E

2014-09-01

Hydrogels based on poly(ethylene glycol) (PEG) are increasingly used in biomedical applications because of their ability to control cell-material interactions by tuning hydrogel physical and biological properties. Evaluation of stability after drying and storage are critical in creating an off-the-shelf biomaterial that functions in vivo according to original specifications. However, there has not been a study that systematically investigates the effects of different drying conditions on hydrogel compositional variables. In the first part of this study, PEG-diacrylate hydrogels underwent common processing procedures (vacuum-drying, lyophilizing, hydrating then vacuum-drying), and the effect of this processing on the mechanical properties and swelling ratios was measured. Significant changes in compressive modulus, tensile modulus, and swelling ratio only occurred for select processed hydrogels. No consistent trends were observed after processing for any of the formulations tested. The effect of storage conditions on cell adhesion and spreading on collagen- and streptococcal collagen-like protein (Scl2-2)-PEG-diacrylamide hydrogels was then evaluated to characterize bioactivity retention after storage. Dry storage conditions preserved bioactivity after 6 weeks of storage; whereas, storage in PBS significantly reduced bioactivity. This loss of bioactivity was attributed to ester hydrolysis of the protein linker, acrylate-PEG-N-hydroxysuccinimide. These studies demonstrate that these processing methods and dry storage conditions may be used to prepare bioactive PEG hydrogel scaffolds with recoverable functionality after storage. © 2013 Wiley Periodicals, Inc.

Preparation and properties of polyvinyl alcohol (PVA) and hydroxylapatite (HA) hydrogels for cartilage tissue engineering.

Science.gov (United States)

Yuan, F; Ma, M; Lu, L; Pan, Z; Zhou, W; Cai, J; Luo, S; Zeng, W; Yin, F

2017-05-20

A novel bioactive hydrogel for cartilage tissue based on polyvinyl alcohol (PVA) and hydroxylapatite (HA) were prepared, the effects of its component contents on the mechanical properties and microstructure of the hydrogel were investigated. The important properties of the scaffold composites, such as density, porosity, compressive modulus and microstructure were studied and analyzed through various measurements and methods. The biodegradability of hydrogel was evaluated by soaking the samples into artificial degradation solution at body temperature (36 - 37 oC) in vitro. Experimental results showed that the PVA/HA hydrogels had a density of 0.572 - 0.683 g/cm3, a porosity of 63.25 - 96.14% and a compressive modulus of 5.62 - 8.24 MP. The HA compound in the hydrogels enhanced the biodegradation significantly and linearly increased the rate of biodegradation by 2.3 - 8.5 %. The compressive modulus of PVA/HA exhibited a linear reduce to 0.86 - 1.53 MP with the time of degradation. The scaffold composites PVA/HA possess a high porosity, decent compressive modulus and good biodegradability. After further optimizing the structure and properties, this composite might be considered as novel hydrogel biomaterials to be applied in the field of cartilage tissue engineering.

Thromboelastometric and platelet responses to silk biomaterials.

Science.gov (United States)

Kundu, Banani; Schlimp, Christoph J; Nürnberger, Sylvia; Redl, Heinz; Kundu, S C

2014-05-13

Silkworm's silk is natural biopolymer with unique properties including mechanical robustness, all aqueous base processing and ease in fabrication into different multifunctional templates. Additionally, the nonmulberry silks have cell adhesion promoting tri-peptide (RGD) sequences, which make it an immensely potential platform for regenerative medicine. The compatibility of nonmulberry silk with human blood is still elusive; thereby, restricts its further application as implants. The present study, therefore, evaluate the haematocompatibility of silk biomaterials in terms of platelet interaction after exposure to nonmulberry silk of Antheraea mylitta using thromboelastometry (ROTEM). The mulberry silk of Bombyx mori and clinically used Uni-Graft W biomaterial serve as references. Shortened clotting time, clot formation times as well as enhanced clot strength indicate the platelet mediated activation of blood coagulation cascade by tested biomaterials; which is comparable to controls.

Swelling, mechanical and friction properties of PVA/PVP hydrogels after swelling in osmotic pressure solution.

Science.gov (United States)

Shi, Yan; Xiong, Dangsheng; Liu, Yuntong; Wang, Nan; Zhao, Xiaoduo

2016-08-01

The potential of polyvinyl alcohol/polyvinylpyrrolidone (PVA/PVP) hydrogels as articular cartilage replacements was in vitro evaluated by using a macromolecule-based solution to mimic the osmotic environment of cartilage tissue. The effects of osmotic pressure solution on the morphology, crystallinity, swelling, mechanical and friction properties of PVA/PVP hydrogels were investigated by swelling them in non-osmotic and osmotic pressure solutions. The results demonstrated that swelling ratio and equilibrium water content were greatly reduced by swelling in osmotic solution, and the swelling process was found to present pseudo-Fickian diffusion character. The crystallization degree of hydrogels after swelling in osmotic solution increased more significantly when it compared with that in non-osmotic solution. After swelling in osmotic solution for 28days, the compressive tangent modulus and storage modulus of hydrogels were significantly increased, and the low friction coefficient was reduced. However, after swelling in the non-osmotic solution, the compressive tangent modulus and friction coefficient of hydrogels were comparable with those of as-prepared hydrogels. The better material properties of hydrogels in vivo than in vitro evaluation demonstrated their potential application in cartilage replacement. Copyright © 2016 Elsevier B.V. All rights reserved.

Synthesis of PVA/PVP hydrogels having two layers by radiation and their physical properties

International Nuclear Information System (INIS)

Nho, Y.C.; Park, K.R.

2002-01-01

Complete text of publication follows. The radiation can induce chemical reaction to modify polymer under even the solid state or in the low temperature. The radiation crosslinking can be easily adjusted by controlling the radiation dose and is reproducible. The finished product contains no residuals of substances required to initiate the chemical crosslinking that can restrict the application possibilities. In these studies, two layer's hydrogel which consisted of urethane membrane and a mixture of polyvinyl alcohol/poly-N-vinylpyrrolidone /glycerin/chitosan was made by gamma-ray irradiation or two steps of 'freezing and thawing' and gamma-ray irradiation for wound dressing. The physical properties such as gelation, water absorptivity, and gel strength were examined to evaluate the hydrogels for wound dressing. Urethane was dissolved in solvent, the urethane solution was poured on the mould, and then dried to make the thin membrane. Hydrophilic polymer solutions were poured on the urethane membranes, they were exposed to gamma irradiation or 'freezing and thawing' and gamma irradiation doses of 25, 35, 50 and 60 kGy to evaluate the physical properties of hydrogels. The physical properties of hydrogels such as gelation and gel strength were improved, and the evaporation speed of water in hydrogel was low when urethane membrane was used

Photoluminescent properties of spider silk coated with Eu-doped nanoceria

Energy Technology Data Exchange (ETDEWEB)

Dmitrović, Svetlana, E-mail: svetlana8@vin.bg.ac.rs [University of Belgrade, Vinča Institute of Nuclear Sciences (Serbia); Nikolić, Marko G.; Jelenković, Branislav [University of Belgrade, Institute of Physics (Serbia); Prekajski, Marija [University of Belgrade, Vinča Institute of Nuclear Sciences (Serbia); Rabasović, Mihailo [University of Belgrade, Institute of Physics (Serbia); Zarubica, Aleksandra [University of Niš, Department of Chemistry, Faculty of Science and Mathematics (Serbia); Branković, Goran [University of Belgrade, Institute for Multidisciplinary Research, Department of Material Science (Serbia); Matović, Branko [University of Belgrade, Vinča Institute of Nuclear Sciences (Serbia)

2017-02-15

Spider dragline silk was coated with pure as well as Eu-doped ceria nanopowders at the room temperature. The treatment was done by immersion of the spider silk mesh into aqueous solutions of cerium nitrate (Ce(NO{sub 3}){sub 3}) and ammonium hydroxide (NH{sub 4}OH). Depending on the relationship between Ce{sup 3+} ion and ammonium hydroxide concentration, coated fibers exhibited a different thickness. Obtained materials were studied by means of FESEM. It was found that ceria nanoparticles of average size of 3 nm were coated along spider thread. X-ray diffraction (XRD) and selected-area electron diffraction (SAED) confirmed crystal nature of nanoparticle coating of spider silk. By using Williamson-Hall plots, crystallite size and strain were estimated. EDS measurement confirmed the presence of Eu in spider-Eu-doped ceria composite, and according to FTIR analysis, the interaction between CeO2 and spider silk was proposed. The morphology of obtained composite was observed by TEM. The photoluminescence emission spectra of spider silk coated with Eu-doped ceria were measured with two different excitations of 385 and 466 nm. The two-photon excited auto-fluorescence of spider silk coated with Eu-doped ceria was detected using a nonlinear laser scanning microscope. Obtained composite has a potential as a fluorescent labeling material in diverse applications.

Photoluminescent properties of spider silk coated with Eu-doped nanoceria

International Nuclear Information System (INIS)

Dmitrović, Svetlana; Nikolić, Marko G.; Jelenković, Branislav; Prekajski, Marija; Rabasović, Mihailo; Zarubica, Aleksandra; Branković, Goran; Matović, Branko

2017-01-01

Spider dragline silk was coated with pure as well as Eu-doped ceria nanopowders at the room temperature. The treatment was done by immersion of the spider silk mesh into aqueous solutions of cerium nitrate (Ce(NO_3)_3) and ammonium hydroxide (NH_4OH). Depending on the relationship between Ce"3"+ ion and ammonium hydroxide concentration, coated fibers exhibited a different thickness. Obtained materials were studied by means of FESEM. It was found that ceria nanoparticles of average size of 3 nm were coated along spider thread. X-ray diffraction (XRD) and selected-area electron diffraction (SAED) confirmed crystal nature of nanoparticle coating of spider silk. By using Williamson-Hall plots, crystallite size and strain were estimated. EDS measurement confirmed the presence of Eu in spider-Eu-doped ceria composite, and according to FTIR analysis, the interaction between CeO2 and spider silk was proposed. The morphology of obtained composite was observed by TEM. The photoluminescence emission spectra of spider silk coated with Eu-doped ceria were measured with two different excitations of 385 and 466 nm. The two-photon excited auto-fluorescence of spider silk coated with Eu-doped ceria was detected using a nonlinear laser scanning microscope. Obtained composite has a potential as a fluorescent labeling material in diverse applications.

Preparation and properties of silk sericin/cellulose cross-linking films

Directory of Open Access Journals (Sweden)

Wang Kunyan

2017-01-01

Full Text Available Silk sericin/cellulose cross-linked films were successfully prepared using glutaraldehyde as cross-linkinger. FTIR was applied to characterize the chemical structure of films. Cross-linked silk sericin film was found the peak intensity of FTIR for cross-linked film decreased markedly compared to pure silk sericin, which indicating cross-linking reaction has been occurred. The increasing value of swelling ratio also indicated the cross-linking has been happened. The cross-linking reaction increased the thermal decomposition temperature.

Graphene oxide and hyperbranched polymer-toughened hydrogels with improved absorption properties and durability

DEFF Research Database (Denmark)

Yu, Yang; De Andrade, Leandro Carvalho Xavier; Fang, Liming

2015-01-01

Hyperbranched polymers or/and graphene oxide nanosheets were used to synthesize poly(acrylic acid)-based hybrid hydrogels with high water absorption ability, excellent mechanical properties, and environmental remediation abilities through a novel one-step, cost-effective, and environmentally...... friendly method. The combination of hyperbranched polymers and graphene oxide nanosheets had synergistic effects on the final hybrid hydrogel, especially on the mechanical behaviors of the hydrogels, with Young's modulus, tensile strength at break and elongation at break increasing by 69, 308, and 848...

Regulation of Silk Material Structure by Temperature-Controlled Water Vapor Annealing

Science.gov (United States)

Hu, Xiao; Shmelev, Karen; Sun, Lin; Gil, Eun-Seok; Park, Sang-Hyug; Cebe, Peggy; Kaplan, David L.

2011-01-01

We present a simple and effective method to obtain refined control of the molecular structure of silk biomaterials through physical temperature-controlled water vapor annealing (TCWVA). The silk materials can be prepared with control of crystallinity, from a low content using conditions at 4°C (alpha-helix dominated silk I structure), to highest content of ~60% crystallinity at 100°C (beta-sheet dominated silk II structure). This new physical approach covers the range of structures previously reported to govern crystallization during the fabrication of silk materials, yet offers a simpler, green chemistry, approach with tight control of reproducibility. The transition kinetics, thermal, mechanical, and biodegradation properties of the silk films prepared at different temperatures were investigated and compared by Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), uniaxial tensile studies, and enzymatic degradation studies. The results revealed that this new physical processing method accurately controls structure, in turn providing control of mechanical properties, thermal stability, enzyme degradation rate, and human mesenchymal stem cell interactions. The mechanistic basis for the control is through the temperature controlled regulation of water vapor, to control crystallization. Control of silk structure via TCWVA represents a significant improvement in the fabrication of silk-based biomaterials, where control of structure-property relationships is key to regulating material properties. This new approach to control crystallization also provides an entirely new green approach, avoiding common methods which use organic solvents (methanol, ethanol) or organic acids. The method described here for silk proteins would also be universal for many other structural proteins (and likely other biopolymers), where water controls chain interactions related to material properties. PMID:21425769

Sequence Identification, Recombinant Production, and Analysis of the Self-Assembly of Egg Stalk Silk Proteins from Lacewing Chrysoperla carnea.

Science.gov (United States)

Neuenfeldt, Martin; Scheibel, Thomas

2017-06-13

Egg stalk silks of the common green lacewing Chrysoperla carnea likely comprise at least three different silk proteins. Based on the natural spinning process, it was hypothesized that these proteins self-assemble without shear stress, as adult lacewings do not use a spinneret. To examine this, the first sequence identification and determination of the gene expression profile of several silk proteins and various transcript variants thereof was conducted, and then the three major proteins were recombinantly produced in Escherichia coli encoded by their native complementary DNA (cDNA) sequences. Circular dichroism measurements indicated that the silk proteins in aqueous solutions had a mainly intrinsically disordered structure. The largest silk protein, which we named ChryC1, exhibited a lower critical solution temperature (LCST) behavior and self-assembled into fibers or film morphologies, depending on the conditions used. The second silk protein, ChryC2, self-assembled into nanofibrils and subsequently formed hydrogels. Circular dichroism and Fourier transform infrared spectroscopy confirmed conformational changes of both proteins into beta sheet rich structures upon assembly. ChryC3 did not self-assemble into any morphology under the tested conditions. Thereby, through this work, it could be shown that recombinant lacewing silk proteins can be produced and further used for studying the fiber formation of lacewing egg stalks.

Dually cross-linked single network poly(acrylic acid) hydrogels with superior mechanical properties and water absorbency.

Science.gov (United States)

Zhong, Ming; Liu, Yi-Tao; Liu, Xiao-Ying; Shi, Fu-Kuan; Zhang, Li-Qin; Zhu, Mei-Fang; Xie, Xu-Ming

2016-06-28

Poly(acrylic acid) (PAA) hydrogels with superior mechanical properties, based on a single network structure with dual cross-linking, are prepared by one-pot free radical polymerization. The network structure of the PAA hydrogels is composed of dual cross-linking: a dynamic and reversible ionic cross-linking among the PAA chains enabled by Fe(3+) ions, and a sparse covalent cross-linking enabled by a covalent cross-linker (Bis). Under deformation, the covalently cross-linked PAA chains remain intact to maintain their original configuration, while the Fe(3+)-enabled ionic cross-linking among the PAA chains is broken to dissipate energy and then recombined. It is found that the mechanical properties of the PAA hydrogels are significantly influenced by the contents of covalent cross-linkers, Fe(3+) ions and water, which can be adjusted within a substantial range and thus broaden the applications of the hydrogels. Meanwhile, the PAA hydrogels have excellent recoverability based on the dynamic and reversible ionic cross-linking enabled by Fe(3+) ions. Moreover, the swelling capacity of the PAA hydrogels is as high as 1800 times in deionized water due to the synergistic effects of ionic and covalent cross-linkings. The combination of balanced mechanical properties, efficient recoverability, high swelling capacity and facile preparation provides a new method to obtain high-performance hydrogels.

Preparation and properties of EDC/NHS mediated crosslinking poly (gamma-glutamic acid)/epsilon-polylysine hydrogels

Energy Technology Data Exchange (ETDEWEB)

Hua, Jiachuan [Key Laboratory of Advanced Textile Composites, Tianjin Polytechnic University, Ministry of Education, Tianjin 300387 (China); School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Li, Zheng, E-mail: lizheng_nx@163.com [Key Laboratory of Advanced Textile Composites, Tianjin Polytechnic University, Ministry of Education, Tianjin 300387 (China); School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Xia, Wen; Yang, Ning; Gong, Jixian [Key Laboratory of Advanced Textile Composites, Tianjin Polytechnic University, Ministry of Education, Tianjin 300387 (China); School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Zhang, Jianfei, E-mail: zhangjianfei1960@126.com [Key Laboratory of Advanced Textile Composites, Tianjin Polytechnic University, Ministry of Education, Tianjin 300387 (China); School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Qiao, Changsheng [Key Laboratory of Industrial Microbiology, Tianjin University of Science and Technology, Ministry of Education, Tianjin 300457 (China)

2016-04-01

In this paper, a novel pH-sensitive poly (amino acid) hydrogel based on poly γ-glutamic acid (γ-PGA) and ε-polylysine (ε-PL) was prepared by carbodiimide (EDC) and N-hydroxysuccinimide (NHS) mediated polymerization. The influence of PGA/PL molar ratio and EDC/NHS concentration on the structure and properties was studied. Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS) proved that hydrogels were crosslinked through amide bond linkage, and the conversion rate of a carboxyl group could reach 96%. Scanning electron microscopy (SEM) results showed a regularly porous structure with 20 μm pore size in average. The gelation time in the crosslink process of PGA/PL hydrogels was within less than 5 min. PGA/PL hydrogels had excellent optical performance that was evaluated by a novel optotype method. Furthermore, PGA/PL hydrogels were found to be pH-sensitive, which could be adjusted to the pH of swelling media intelligently. The terminal pH of swelling medium could be controlled at 5 ± 1 after equilibrium when the initial pH was within 3–11. The swelling kinetics was found to follow a Voigt model in deionized water but a pseudo-second-order model in normal saline and phosphate buffer solution, respectively. The differential swelling degrees were attributed to the swelling theory based on the different ratio of –COOH/–NH{sub 2} and pore size in hydrogels. The results of mechanical property indicated that PGA/PL hydrogels were soft and elastic. Moreover, PGA/PL hydrogels exhibited excellent biocompatibility by cell proliferation experiment. PGA/PL hydrogels could be degraded in PBS solution and the degradation rate was decreased with the increase of the molar ratio of PL. Considering the simple preparation process and pH-sensitive property, these PGA/PL hydrogels might have high potential for use in medical and clinical fields. - Highlights: • We prepared a biocompatible and degradable poly amino acids hydrogel via EDC

Purification and some properties of G-factor from the silk gland of silkworm

International Nuclear Information System (INIS)

Taira, Hideharu; Ejiri, Shin-ichiro; Shimura, Kensuke

1972-01-01

Purification of G-factor from the silk gland of silkworms and some of its properties have been studied in comparison with the G-factor from E. coli and rat liver transferase II. In the experiment, GTP-γ- 32 P was prepared from GDP and 32 Pi by photophosphorylation with spinach chloroplasts, and purified by Dowex-1 chromatography. The purified G-factor was homogeneous on disc gel electrophoresis. Molecular weight of 80,000 was estimated from a calibrated Sephadex G-200 column. The purified G-factor exhibited uncoupled ribosome-dependent GTPase activity, and was inhibited by fusidic acid, SH inhibitor, and diphtheria toxin plus NAD. The G-factor from E. coli and that from the silk gland were not interchangeable in GTPase reaction. (Yamanoto, Y.)

Purification and some properties of G-factor from the silk gland of silkworm

Energy Technology Data Exchange (ETDEWEB)

Taira, H; Ejiri, S I; Shimura, K [Tohoku Univ., Sendai (Japan). Faculty of Agriculture

1972-12-01

Purification of G-factor from the silk gland of silkworms and some of its properties have been studied in comparison with the G-factor from E. coli and rat liver transferase II. In the experiment, GTP-..gamma..-/sup 32/P was prepared from GDP and /sup 32/Pi by photophosphorylation with spinach chloroplasts, and purified by Dowex-1 chromatography. The purified G-factor was homogeneous on disc gel electrophoresis. Molecular weight of 80,000 was estimated from a calibrated Sephadex G-200 column. The purified G-factor exhibited uncoupled ribosome-dependent GTPase activity, and was inhibited by fusidic acid, SH inhibitor, and diphtheria toxin plus NAD. The G-factor from E. coli and that from the silk gland were not interchangeable in GTPase reaction.

MMP-sensitive PEG diacrylate hydrogels with spatial variations in matrix properties stimulate directional vascular sprout formation.

Directory of Open Access Journals (Sweden)

Michael V Turturro

Full Text Available The spatial presentation of immobilized extracellular matrix (ECM cues and matrix mechanical properties play an important role in directed and guided cell behavior and neovascularization. The goal of this work was to explore whether gradients of elastic modulus, immobilized matrix metalloproteinase (MMP-sensitivity, and YRGDS cell adhesion ligands are capable of directing 3D vascular sprout formation in tissue engineered scaffolds. PEGDA hydrogels were engineered with mechanical and biofunctional gradients using perfusion-based frontal photopolymerization (PBFP. Bulk photopolymerized hydrogels with uniform mechanical properties, degradation, and immobilized biofunctionality served as controls. Gradient hydrogels exhibited an 80.4% decrease in elastic modulus and a 56.2% decrease in immobilized YRGDS. PBFP hydrogels also demonstrated gradients in hydrogel degradation with degradation times ranging from 10-12 hours in the more crosslinked regions to 4-6 hours in less crosslinked regions. An in vitro model of neovascularization, composed of co-culture aggregates of endothelial and smooth muscle cells, was used to evaluate the effect of these gradients on vascular sprout formation. Aggregate invasion in gradient hydrogels occurred bi-directionally with sprout alignment observed in the direction parallel to the gradient while control hydrogels with homogeneous properties resulted in uniform invasion. In PBFP gradient hydrogels, aggregate sprout length was found to be twice as long in the direction parallel to the gradient as compared to the perpendicular direction after three weeks in culture. This directionality was found to be more prominent in gradient regions of increased stiffness, crosslinked MMP-sensitive peptide presentation, and immobilized YRGDS concentration.

Improved strength of silk fibers in Bombyx mori trimolters induced by an anti-juvenile hormone compound.

Science.gov (United States)

Guo, Kaiyu; Dong, Zhaoming; Zhang, Yan; Wang, Dandan; Tang, Muya; Zhang, Xiaolu; Xia, Qingyou; Zhao, Ping

2018-05-01

Bombyx mori silk fibers with thin diameters have advantages of lightness and crease-resistance. Many studies have used anti-juvenile hormones to induce trimolters in order to generate thin silk; however, there has been comparatively little analysis of the morphology, structure and mechanical properties of trimolter silk. This study induced two kinds of trimolters by appling topically anti-juvenile hormones and obtained thin diameter silk. Scanning electron microscope (SEM), FTIR analysis, tensile mechanical testing, chitin staining were used to reveal that the morphology, conformation and mechanical property of the trimolter silk. Cocoon of trimolters were highly densely packed by thinner fibers and thus had small apertures. We found that the conformation of trimolter silk fibroin changed and formed more β-sheet structures. In addition, analysis of mechanical parameters yielded a higher Young's modulus and strength in trimolter silk than in the control. By chitin staining of silk gland, we postulated that the mechanical properties of trimolters' silk was enhanced greatly during to the structural changes of silk gland. We induced trimolters by anti-juvenile hormones and the resulting cocoons were more closely packed and had smaller silk fiber diameters. We found that the conformation of trimolters silk fibroin had a higher content of β-sheet structures and better mechanical properties. Our study revealed the structures and mechanical properties of trimolter silk, and provided a valuable reference to improve silk quality by influencing molting in silkworms. Copyright © 2018 Elsevier B.V. All rights reserved.

Spider silk reinforced by graphene or carbon nanotubes

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Lepore, Emiliano; Bosia, Federico; Bonaccorso, Francesco; Bruna, Matteo; Taioli, Simone; Garberoglio, Giovanni; Ferrari, Andrea C.; Pugno, Nicola Maria

2017-09-01

Spider silk has promising mechanical properties, since it conjugates high strength (~1.5 GPa) and toughness (~150 J g-1). Here, we report the production of silk incorporating graphene and carbon nanotubes by spider spinning, after feeding spiders with the corresponding aqueous dispersions. We observe an increment of the mechanical properties with respect to pristine silk, up to a fracture strength ~5.4 GPa and a toughness modulus ~1570 J g-1. This approach could be extended to other biological systems and lead to a new class of artificially modified biological, or ‘bionic’, materials.

Bioprospecting finds the toughest biological material: extraordinary silk from a giant riverine orb spider.

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Ingi Agnarsson

Full Text Available BACKGROUND: Combining high strength and elasticity, spider silks are exceptionally tough, i.e., able to absorb massive kinetic energy before breaking. Spider silk is therefore a model polymer for development of high performance biomimetic fibers. There are over 41,000 described species of spiders, most spinning multiple types of silk. Thus we have available some 200,000+ unique silks that may cover an amazing breadth of material properties. To date, however, silks from only a few tens of species have been characterized, most chosen haphazardly as model organisms (Nephila or simply from researchers' backyards. Are we limited to 'blindly fishing' in efforts to discover extraordinary silks? Or, could scientists use ecology to predict which species are likely to spin silks exhibiting exceptional performance properties? METHODOLOGY: We examined the biomechanical properties of silk produced by the remarkable Malagasy 'Darwin's bark spider' (Caerostris darwini, which we predicted would produce exceptional silk based upon its amazing web. The spider constructs its giant orb web (up to 2.8 m(2 suspended above streams, rivers, and lakes. It attaches the web to substrates on each riverbank by anchor threads as long as 25 meters. Dragline silk from both Caerostris webs and forcibly pulled silk, exhibits an extraordinary combination of high tensile strength and elasticity previously unknown for spider silk. The toughness of forcibly silked fibers averages 350 MJ/m(3, with some samples reaching 520 MJ/m(3. Thus, C. darwini silk is more than twice tougher than any previously described silk, and over 10 times better than Kevlar®. Caerostris capture spiral silk is similarly exceptionally tough. CONCLUSIONS: Caerostris darwini produces the toughest known biomaterial. We hypothesize that this extraordinary toughness coevolved with the unusual ecology and web architecture of these spiders, decreasing the likelihood of bridgelines breaking and collapsing the web

Silk Electrogel Rheology

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Tabatabai, A. P.; Urbach, J. S.; Blair, D. L.; Kaplan, D. L.

2014-03-01

We present experimental results on the rheology on electrogels derived from aqueous solutions of reconstituted Bombyx Mori silk fibroin protein. Through electrochemistry, the silk protein solution develops local pH changes resulting in the assembly of protein into a weak gel. We determine the physical properties of the electrogels by performing rheology and observe that they exhibit the characteristics of a crosslinked biopolymer network. Interestingly, we find that these silk gels exhibit linear elasticity over a range of up to two orders of magnitude larger than most crosslinked biopolymer networks. Moreover, the nonlinear rheology exhibits a strain-stiffening behavior that is fundamentally different than the strain-stiffening observed in crosslinked biopolymers. Through rheological techniques we aim to understand this distinctive material that cannot be explained by current polymeric models. This work is supported by a grant from the AFOSR FA9550-07-1-0130.

Tragacanth gum/nano silver hydrogel on cotton fabric: In-situ synthesis and antibacterial properties.

Science.gov (United States)

Montazer, M; Keshvari, A; Kahali, P

2016-12-10

This paper is mainly focused on introducing cotton fabric with hydrogel and antimicrobial properties using Tragacanth gum as a natural polymer with hydrogel properties, silver nitrate as silver precursor, citric acid as a cross-linking agent and sodium hypophosphite as catalyst. The water absorption behavior of the treated fabrics was investigated with moisture regain, water retention, drying time of wetted fabric at room condition and vertical wicking tests. Antibacterial properties of the samples were evaluated against Escherichia coli and Staphylococcous aureus. The SEM pictures confirmed formation of nano silver and hydrogel layer on the fabric surface and XRD performed the crystal and particle size of the nano silver. The chemical structure of the fabric samples was identified with FTIR spectra. The central composite design (CCD) was used for statistical modelling, evaluated effective parameters and created optimum conditions. The treated cotton fabrics showed good water absorption properties along with reasonable antibacterial effectiveness. Copyright © 2016 Elsevier Ltd. All rights reserved.

Effect of Crosslinking Agent Concentration on the Properties of Unmedicated Hydrogels

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Rachel Shet Hui Wong

2015-09-01

Full Text Available Novel polyethylene oxide (PEO hydrogel films were synthesized via UV crosslinking with varying concentrations of pentaerythritol tetra-acrylate (PETRA as crosslinking agent. The aim was to study the effects of the crosslinking agent on the material properties of hydrogel films intended for dermatological applications. Fabricated film samples were characterized using swelling studies, scanning electron microscopy, tensile testing and rheometry. Films showed rapid swelling and high elasticity. The increase of PETRA concentration resulted in significant increase in the gel fraction and crosslinking density (ρc, while causing a significant decrease in the equilibrium water content (EWC, average molecular weight between crosslinks (\\({\\overline{M}}_{c}\\, and mesh size (ζ of films. From the scanning electron microscopy, cross-linked PEO hydrogel network appeared as cross-linked mesh-like structure with interconnected micropores. Rheological studies showed PEO films required a minimum of 2.5% w/w PETRA to form stable viscoelastic solid gels. Preliminary studies concluded that a minimum of 2.5% w/w PETRA is required to yield films with desirable properties for skin application.

Novel antifouling self-healing poly(carboxybetaine methacrylamide-co-HEMA) nanocomposite hydrogels with superior mechanical properties

NARCIS (Netherlands)

Kostina, Nina Yu.; Sharifi, Shahriar; Pereira, Andres de los Santos; Michalek, Jiri; Grijpma, Dirk W.; Rodriguez-Emmenegger, Cesar

2013-01-01

Novel antifouling highly wettable hydrogels with superior mechanical and self-healing properties are presented. Hydrogels were prepared by UV-initiated copolymerisation of non-fouling zwitterionic carboxybetaine methacrylamide (CBMAA-3) and 2-hydroxyethyl methacrylate (HEMA) in the presence of

Synthetic Spider Silk Production on a Laboratory Scale

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Hsia, Yang; Gnesa, Eric; Pacheco, Ryan; Kohler, Kristin; Jeffery, Felicia; Vierra, Craig

2012-01-01

As society progresses and resources become scarcer, it is becoming increasingly important to cultivate new technologies that engineer next generation biomaterials with high performance properties. The development of these new structural materials must be rapid, cost-efficient and involve processing methodologies and products that are environmentally friendly and sustainable. Spiders spin a multitude of different fiber types with diverse mechanical properties, offering a rich source of next generation engineering materials for biomimicry that rival the best manmade and natural materials. Since the collection of large quantities of natural spider silk is impractical, synthetic silk production has the ability to provide scientists with access to an unlimited supply of threads. Therefore, if the spinning process can be streamlined and perfected, artificial spider fibers have the potential use for a broad range of applications ranging from body armor, surgical sutures, ropes and cables, tires, strings for musical instruments, and composites for aviation and aerospace technology. In order to advance the synthetic silk production process and to yield fibers that display low variance in their material properties from spin to spin, we developed a wet-spinning protocol that integrates expression of recombinant spider silk proteins in bacteria, purification and concentration of the proteins, followed by fiber extrusion and a mechanical post-spin treatment. This is the first visual representation that reveals a step-by-step process to spin and analyze artificial silk fibers on a laboratory scale. It also provides details to minimize the introduction of variability among fibers spun from the same spinning dope. Collectively, these methods will propel the process of artificial silk production, leading to higher quality fibers that surpass natural spider silks. PMID:22847722

Water swelling properties of the electron beam irradiated PVA-g-AAc hydrogels

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Wang, Qingguo, E-mail: qwang@qust.edu.cn [Key Laboratory of Rubber-Plastics of Ministry of Education, Qingdao University of Science and Technology, Qingdao 266042 (China); Shandong Provincial Key Laboratory of Rubber-Plastics, Qingdao 266042 (China); Zhou, Xue; Zeng, Jinxia; Wang, Jizeng [Key Laboratory of Rubber-Plastics of Ministry of Education, Qingdao University of Science and Technology, Qingdao 266042 (China)

2016-02-01

In this paper, the electron beam irradiation technology being more suitable for the industry application is explored to fabricate the acrylic acid (AAc) monomer-grafted polyvinyl alcohol (PVA-g-AAc) hydrogels. ATR-IR spectra of the PVA-g-AAc hydrogels shows an obvious absorption peak of the −C=O group at 1701 cm{sup −1}, indicating that the AAc monomers were grafted onto the PVA macromolecules. This paper also studied some effects of the mass ratio of PVA/AAc, pH of buffer solution and irradiation dosage on the water swelling properties of the electron beam irradiated PVA-g-AAc hydrogels. The water swelling ratio of PVA-g-AAc hydrogels decreases with increased irradiation dosage and mass ratio of PVA/AAc, whereas swelling ratio increases with increased pH of buffer solution and soaking time. The water-swelling behavior of PVA-g-AAc hydrogels occurred easily in an alkaline environment, particularly in a buffer solution with pH 9.2. Both PVA-g-AAc hydrogels (PVA/AAc = 1/5, w/w) irradiated with 5 kilogray (kGy) and PVA-g-AAc hydrogels (PVA/AAc = 1/1, w/w) irradiated with 15 kGy could easily absorb water and lead to high water swelling ratios (up to about 600%), which are potential candidates to meet the requirements for some biomedical applications.

Hydrogels for lung tissue engineering: Biomechanical properties of thin collagen-elastin constructs.

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Dunphy, Siobhán E; Bratt, Jessica A J; Akram, Khondoker M; Forsyth, Nicholas R; El Haj, Alicia J

2014-10-01

In this study, collagen-elastin constructs were prepared with the aim of producing a material capable of mimicking the mechanical properties of a single alveolar wall. Collagen has been used in a wide range of tissue engineering applications; however, due to its low mechanical properties its use is limited to non load-bearing applications without further manipulation using methods such as cross-linking or mechanical compression. Here, it was hypothesised that the addition of soluble elastin to a collagen hydrogel could improve its mechanical properties. Hydrogels made from collagen only and collagen plus varying amounts elastin were prepared. Young׳s modulus of each membrane was measured using the combination of a non-destructive indentation and a theoretical model previously described. An increase in Young׳s modulus was observed with increasing concentration of elastin. The use of non-destructive indentation allowed for online monitoring of the elastic moduli of cell-seeded constructs over 8 days. The addition of lung fibroblasts into the membrane increased the stiffness of the hydrogels further and cell-seeded collagen hydrogels were found to have a stiffness equal to the theoretical value for a single alveolar wall (≈5kPa). Through provision of some of the native extracellular matrix components of the lung parenchyma these scaffolds may be able to provide an initial building block toward the regeneration of new functional lung tissue. Copyright © 2014 Elsevier Ltd. All rights reserved.

Structural and biological properties of thermosensitive chitosan-graphene hybrid hydrogels for sustained drug delivery applications.

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Saeednia, Leyla; Yao, Li; Berndt, Marcus; Cluff, Kim; Asmatulu, Ramazan

2017-09-01

Chitosan has the ability to make injectable thermosensitive hydrogels which has been highly investigated for drug delivery applications. The addition of nanoparticles is one way to increase the mechanical strength of thermosensitive chitosan hydrogel and subsequently and control the burst release of drug. Graphene nanoparticles have shown unique mechanical, optical and electrical properties which can be exploited for biomedical applications, especially in drug delivery. This study, have focused on the mechanical properties of a thermosensitive and injectable hybrid chitosan hydrogel incorporated with graphene nanoparticles. Scanning electron microscope (SEM), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and X-ray diffraction (XRD) have been used for morphological and chemical characterization of graphene infused chitosan hydrogels. The cell viability and cytotoxicity of graphene-contained hydrogels were analyzed using the alamarBlue ® technique. In-vitro methotrexate (MTX) release was investigated from MTX-loaded hybrid hydrogels as well. As a last step, to evaluate their efficiency as a cancer treatment delivery system, an in vitro anti-tumor test was also carried out using MCF-7 breast cancer cell lines. Results confirmed that a thermosensitive chitosan-graphene hybrid hydrogel can be used as a potential breast cancer therapy system for controlled delivery of methotrexate. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 105A: 2381-2390, 2017. © 2017 Wiley Periodicals, Inc.

Highly water-absorbing silk yarn with interpenetrating network via in situ polymerization.

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Lee, Ka I; Wang, Xiaowen; Guo, Xia; Yung, Ka-Fu; Fei, Bin

2017-02-01

Silk was modified via in situ polymerization of two monomers acrylamide and sodium acrylate by swelling in an effective LiBr dissolution system. Swelling of natural silks in LiBr solutions of low concentration was clearly observed under optical microscope, and their conformational changes were revealed by X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. Dissolution tests and FTIR spectra of these modified silks suggested the presence of interpenetrating network of polyacrylamide and poly(sodium acrylate) in the silk yarns. These modified silks exhibited superior water absorption to that of raw silk and greatly improved mechanical properties in both dry and wet states. These novel modified silks also showed low cytotoxicity towards skin keratinocytes, having potential applications in biomedical textiles. This modification method by in situ polymerization after swelling in LiBr provides a new route to highly enhance the properties and performance of silk for various applications. Copyright © 2016 Elsevier B.V. All rights reserved.

Effect of Drug Loading Method and Drug Physicochemical Properties on the Material and Drug Release Properties of Poly (Ethylene Oxide Hydrogels for Transdermal Delivery

Directory of Open Access Journals (Sweden)

Rachel Shet Hui Wong

2017-07-01

Full Text Available Novel poly (ethylene oxide (PEO hydrogel films were synthesized via UV cross-linking with pentaerythritol tetra-acrylate (PETRA as cross-linking agent. The purpose of this work was to develop a novel hydrogel film suitable for passive transdermal drug delivery via skin application. Hydrogels were loaded with model drugs (lidocaine hydrochloride (LID, diclofenac sodium (DIC and ibuprofen (IBU via post-loading and in situ loading methods. The effect of loading method and drug physicochemical properties on the material and drug release properties of medicated film samples were characterized using scanning electron microscopy (SEM, swelling studies, differential scanning calorimetry (DSC, fourier transform infrared spectroscopy (FT-IR, tensile testing, rheometry, and drug release studies. In situ loaded films showed better drug entrapment within the hydrogel network and also better polymer crystallinity. High drug release was observed from all studied formulations. In situ loaded LID had a plasticizing effect on PEO hydrogel, and films showed excellent mechanical properties and prolonged drug release. The drug release mechanism for the majority of medicated PEO hydrogel formulations was determined as both drug diffusion and polymer chain relaxation, which is highly desirable for controlled release formulations.

Flame retardant and hydrophobic properties of novel sol-gel derived phytic acid/silica hybrid organic-inorganic coatings for silk fabric

Science.gov (United States)

Cheng, Xian-Wei; Liang, Cheng-Xi; Guan, Jin-Ping; Yang, Xu-Hong; Tang, Ren-Cheng

2018-01-01

In this work, a novel phosphorus-rich hybrid organic-inorganic silica coating for improving the flame retardancy of silk fabric was prepared using naturally occurring phytic acid as phosphorus precursor and catalyst for the hydrolysis of tetraethoxysilane. In addition, three silane coupling agents, namely 3-aminopropyldimethoxymethylsilane, 3-chloropropyltrimethoxysilane and 3-methacryloxypropyltrimethoxysilane, were added in the hybrid sol as cross-linkers with the aim of developing hydrophobic coatings and improving the washing durability of the treated silk fabric. The condensation degree of the hybrid sol was characterized by solid-state 29Si nuclear magnetic resonance spectroscopy. The flammability and thermal degradation properties of the treated silk fabrics were determined in terms of limiting oxygen index, vertical burning, pyrolysis combustion flow calorimetry and thermogravimetric analyses. The surface morphology and hydrophobicity of the treated silk fabrics were evaluated by scanning electron microscopy, atomic force microscopy and water contact angle tests. The flammability tests revealed that the silicon sol could endow silk fabric with excellent flame retardancy when doped with phytic acid, and the treated silk fabrics self-extinguished immediately when the ignition source was removed. The silk fabrics treated with the modified hybrid sols exhibited hydrophobic surface and also better durability to washing.

Preparation and properties of hydrogels of PVA/PVP/chitosan by radiation

International Nuclear Information System (INIS)

Nho, Y. C.; Park, K. R.

2001-01-01

The radiation can induce chemical reaction to modify polymer under even the solid condition or in the low temperature. The radiation crosslinking can be easily adjusted and is easily reproducible by controlling the radiation dose. The finished product contains no residuals of substances required to initiate the chemical crosslinking which can restrict the application possibilities. In these studies, hydrogels from a mixture of chitosan and polyvinyl alcohol(PVA)/Poly-N-vinylpyrrolidone(PVP) were made by 'freezing and thawing', or gamma-ray irradiation or two steps of 'freezing and thawing', and gamma-ray irradiation or two steps of 'freezing and thawing' and gamma-ray irradiation for wound dressing. The mechanical properties such as gelation, water absorptivity, and gel strength were examined to evaluate the hydrogels for wound dressing. The composition of PVA:PVP was 60:40, PVA/PVP: chitosan ratio was in the range of 9:1 -7:3, and the solid concentration of PVA/PVP/chitosan solution was 15wt%. Gamma irradiation doses of 25, 35, 50, 60 and 70kGy, respectively were exposed to a mixture of PVA/PVP/chitosan to evaluate the effect of irradiation dose on the mechanical properties of hydrogels. Water-soluble chitosan was used to in this experiment. The mechanical properties of hydrogels such as gelation and gel strength was higher when two steps of 'freezing and thawing' and irradiation were used than only 'freezing and thawing' was utilized. Gel content was influenced slightly by PVA/PVP:chitosan composition and irradiation dose, but swelling was done greatly by them. Swelling percent was much increased as the composition of chitosan in PVA/PVP/chitosan increased

Alginate-Collagen Fibril Composite Hydrogel

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Mahmoud Baniasadi

2015-02-01

Full Text Available We report on the synthesis and the mechanical characterization of an alginate-collagen fibril composite hydrogel. Native type I collagen fibrils were used to synthesize the fibrous composite hydrogel. We characterized the mechanical properties of the fabricated fibrous hydrogel using tensile testing; rheometry and atomic force microscope (AFM-based nanoindentation experiments. The results show that addition of type I collagen fibrils improves the rheological and indentation properties of the hydrogel.

Multifunctional silk-heparin biomaterials for vascular tissue engineering applications

Science.gov (United States)

Seib, F. Philipp; Herklotz, Manuela; Burke, Kelly A.; Maitz, Manfred F.; Werner, Carsten; Kaplan, David L.

2013-01-01

Over the past 30 years, silk has been proposed for numerous biomedical applications that go beyond its traditional use as a suture material. Silk sutures are well tolerated in humans, but the use of silk for vascular engineering applications still requires extensive biocompatibility testing. Some studies have indicated a need to modify silk to yield a hemocompatible surface. This study examined the potential of low molecular weight heparin as a material for refining silk properties by acting as a carrier for vascular endothelial growth factor (VEGF) and improving silk hemocompatibility. Heparinized silk showed a controlled VEGF release over 6 days; the released VEGF was bioactive and supported the growth of human endothelial cells. Silk samples were then assessed using a humanized hemocompatibility system that employs whole blood and endothelial cells. The overall thrombogenic response for silk was very low and similar to the clinical reference material polytetrafluoroethylene. Despite an initial inflammatory response to silk, apparent as complement and leukocyte activation, the endothelium was maintained in a resting, anticoagulant state. The low thrombogenic response and the ability to control VEGF release support the further development of silk for vascular applications. PMID:24099708

Microscale characterization of the viscoelastic properties of hydrogel biomaterials using dual-mode ultrasound elastography.

Science.gov (United States)

Hong, Xiaowei; Stegemann, Jan P; Deng, Cheri X

2016-05-01

Characterization of the microscale mechanical properties of biomaterials is a key challenge in the field of mechanobiology. Dual-mode ultrasound elastography (DUE) uses high frequency focused ultrasound to induce compression in a sample, combined with interleaved ultrasound imaging to measure the resulting deformation. This technique can be used to non-invasively perform creep testing on hydrogel biomaterials to characterize their viscoelastic properties. DUE was applied to a range of hydrogel constructs consisting of either hydroxyapatite (HA)-doped agarose, HA-collagen, HA-fibrin, or preosteoblast-seeded collagen constructs. DUE provided spatial and temporal mapping of local and bulk displacements and strains at high resolution. Hydrogel materials exhibited characteristic creep behavior, and the maximum strain and residual strain were both material- and concentration-dependent. Burger's viscoelastic model was used to extract characteristic parameters describing material behavior. Increased protein concentration resulted in greater stiffness and viscosity, but did not affect the viscoelastic time constant of acellular constructs. Collagen constructs exhibited significantly higher modulus and viscosity than fibrin constructs. Cell-seeded collagen constructs became stiffer with altered mechanical behavior as they developed over time. Importantly, DUE also provides insight into the spatial variation of viscoelastic properties at sub-millimeter resolution, allowing interrogation of the interior of constructs. DUE presents a novel technique for non-invasively characterizing hydrogel materials at the microscale, and therefore may have unique utility in the study of mechanobiology and the characterization of hydrogel biomaterials. Copyright © 2016 Elsevier Ltd. All rights reserved.

IPN hydrogel nanocomposites based on agarose and ZnO with antifouling and bactericidal properties

Energy Technology Data Exchange (ETDEWEB)

Wang, Jingjing, E-mail: jjwang1@hotmail.com; Hu, Hongkai; Yang, Zhonglin; Wei, Jun; Li, Juan

2016-04-01

Nanocomposite hydrogels with interpenetrating polymer network (IPN) structure based on poly(ethylene glycol) methyl ether methacrylate modified ZnO (ZnO-PEGMA) and 4-azidobenzoic agarose (AG-N{sub 3}) were prepared by a one-pot strategy under UV irradiation. The hydrogels exhibited a highly macroporous spongelike structure, and the pore size decreased with the increase of the ZnO-PEGMA content. Due to the entanglement and favorable interactions between the two crosslinked networks, the IPN hydrogels exhibited excellent mechanical strength and light transmittance. The maximum compressive and tensile strengths of the IPN hydrogels reached 24.8 and 1.98 MPa respectively. The transparent IPN hydrogels transmitted more than 85% of visible light at all wavelengths (400–800 nm). The IPN hydrogels exhibited anti-adhesive property towards Gram-negative Escherichia coli (E. coli) and Gram-positive Staphylococcus aureus (S. aureus), and the bactericidal activity increased with the ZnO-PEGMA content. The incorporation of ZnO-PEGMA did not reduce the biocompatibility of the IPN hydrogels and all the IPN nanocomposites showed negligible cytotoxicity. The present study not only provided a facile method for preparing hydrogel nanocomposites with IPN structure but also developed a new hydrogel material which might be an excellent candidate for wound dressings. - Highlights: • IPN hydrogel nanocomposites were prepared by a one-pot strategy. • The maximum compressive and tensile strengths reached 24.8 and 1.98 MPa. • IPN hydrogels displayed excellent antibacterial activity and cytocompatibility. • This study provided a facile method for preparing IPN hydrogel nanocomposites.

Enhanced stiffness of silk-like fibers by loop formation in the corona leads to stronger gels.

Science.gov (United States)

Rombouts, Wolf H; Domeradzka, Natalia E; Werten, Marc W T; Leermakers, Frans A M; de Vries, Renko J; de Wolf, Frits A; van der Gucht, Jasper

2016-11-01

We study the self-assembly of protein polymers consisting of a silk-like block flanked by two hydrophilic blocks, with a cysteine residue attached to the C-terminal end. The silk blocks self-assemble to form fibers while the hydrophilic blocks form a stabilizing corona. Entanglement of the fibers leads to the formation of hydrogels. Under oxidizing conditions the cysteine residues form disulfide bridges, effectively connecting two corona chains at their ends to form a loop. We find that this leads to a significant increase in the elastic modulus of the gels. Using atomic force microscopy, we show that this stiffening is due to an increase of the persistence length of the fibers. Self-consistent-field calculations indicate a slight decrease of the lateral pressure in the corona upon loop formation. We argue that this small decrease in the repulsive interactions affects the stacking of the silk-like blocks in the core, resulting in a more rigid fiber. © 2016 Wiley Periodicals, Inc.

Dynamic compressive properties and failure mechanism of glass fiber reinforced silica hydrogel

International Nuclear Information System (INIS)

Yang Jie; Li Shukui; Yan Lili; Huo Dongmei; Wang Fuchi

2010-01-01

The dynamic compressive properties of glass fiber reinforced silica (GFRS) hydrogel were investigated using a spilt Hopkinson pressure bar. Failure mechanism of GFRS hydrogel was studied by scanning electron microscopy (SEM). Result showed that dynamic compressive stresses were much higher than the quasi-static compressive stresses at the same strain. The dynamic compressive strength was directly proportional to the strain rate with same sample dimensions. The dynamic compressive strength was directly proportional to the sample basal area at same strain rate. Dynamic compressive failure strain was small. At high strain rates, glass fibers broke down and separated from the matrix, pores shrank rapidly. Failure resulted from the increase of lateral tensile stress in hydrogel under dynamic compression.

Invited review current progress and limitations of spider silk for biomedical applications.

Science.gov (United States)

Widhe, Mona; Johansson, Jan; Hedhammar, My; Rising, Anna

2012-06-01

Spider silk is a fascinating material combining remarkable mechanical properties with low density and biodegradability. Because of these properties and historical descriptions of medical applications, spider silk has been proposed to be the ideal biomaterial. However, overcoming the obstacles to produce spider silk in sufficient quantities and in a manner that meets regulatory demands has proven to be a difficult task. Also, there are relatively few studies of spider silk in biomedical applications available, and the methods and materials used vary a lot. Herein we summarize cell culture- and in vivo implantation studies of natural and synthetic spider silk, and also review the current status and future challenges in the quest for a large scale production of spider silk for medical applications. Copyright © 2011 Wiley Periodicals, Inc.

Silk I and Silk II studied by fast scanning calorimetry

Energy Technology Data Exchange (ETDEWEB)

Cebe, Peggy; Partlow, Benjamin P.; Kaplan, David L.; Wurm, Andreas; Zhuravlev, Evgeny; Schick, Christoph

2017-06-01

Using fast scanning calorimetry (FSC), we investigated the glass transition and crystal melting of samples of B. mori silk fibroin containing Silk I and/or Silk II crystals. Due to the very short residence times at high temperatures during such measurements, thermal decomposition of silk protein can be significantly suppressed. FSC was performed at 2000 K/s using the Mettler Flash DSC1 on fibroin films with masses around 130–270 ng. Films were prepared with different crystalline fractions (ranging from 0.26 to 0.50) and with different crystal structures (Silk I, Silk II, or mixed) by varying the processing conditions. These included water annealing at different temperatures, exposure to 50% MeOH in water, or autoclaving. The resulting crystal structure was examined using wide angle X-ray scattering. Degree of crystallinity was evaluated from Fourier transform infrared (FTIR) spectroscopy and from analysis of the heat capacity increment at the glass transition temperature. Silk fibroin films prepared by water annealing at 25 °C were the least crystalline and had Silk I structure. FTIR and FSC studies showed that films prepared by autoclaving or 50% MeOH exposure were the most crystalline and had Silk II structure. Intermediate crystalline fraction and mixed Silk I/Silk II structures were found in films prepared by water annealing at 37 °C. FSC results indicate that Silk II crystals exhibit endotherms of narrower width and have higher mean melting temperature Tm(II) = 351 ± 2.6 °C, compared to Silk I crystals which melt at Tm(I) = 292 ± 3.8 °C. Films containing mixed Silk I/Silk II structure showed two clearly separated endothermic peaks. Evidence suggests that the two types of crystals melt separately and do not thermally interconvert on the extremely short time scale (0.065 s between onset and end of melting) of the FSC experiment.

Osteoinductive recombinant silk fusion proteins for bone regeneration.

Science.gov (United States)

Dinjaski, Nina; Plowright, Robyn; Zhou, Shun; Belton, David J; Perry, Carole C; Kaplan, David L

2017-02-01

Protein polymers provide a unique opportunity for tunable designs of material systems due to the genetic basis of sequence control. To address the challenge of biomineralization interfaces with protein based materials, we genetically engineered spider silks to design organic-inorganic hybrid systems. The spider silk inspired domain (SGRGGLGGQG AGAAAAAGGA GQGGYGGLGSQGT) 15 served as an organic scaffold to control material stability and to allow multiple modes of processing, whereas the hydroxyapatite binding domain VTKHLNQISQSY (VTK), provided control over osteogenesis. The VTK domain was fused either to the N-, C- or both terminals of the spider silk domain to understand the effect of position on material properties and mineralization. The addition of the VTK domain to silk did not affect the physical properties of the silk recombinant constructs, but it had a critical role in the induction of biomineralization. When the VTK domain was placed on both the C- and N-termini the formation of crystalline hydroxyapatite was significantly increased. In addition, all of the recombinant proteins in film format supported the growth and proliferation of human mesenchymal stem cells (hMSCs). Importantly, the presence of the VTK domain enhanced osteoinductive properties up to 3-fold compared to the control (silk alone without VTK). Therefore, silk-VTK fusion proteins have been shown suitable for mineralization and functionalization for specific biomedical applications. Organic-inorganic interfaces are integral to biomaterial functions in many areas of repair and regeneration. Several protein polymers have been investigated for this purpose. Despite their success the limited options to fine-tune their material properties, degradation patterns and functionalize them for each specific biomedical application limits their application. Various studies have shown that the biological performance of such proteins can be improved by genetic engineering. The present study provides data

Silk Composite with a Fluoropolymer as a Water-Resistant Protein-Based Material

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Keiji Numata

2018-04-01

Full Text Available Silk-based materials are water-sensitive and show different physical properties at different humidities and under wet/dry conditions. To overcome the water sensitivity of silk-based materials, we developed a silk composite material with a fluoropolymer. Blending and coating the silk protein-based materials, such as films and textiles, with the fluoropolymer enhanced the surface hydrophobicity, water vapor barrier properties, and size stability during shrinkage tests. This material design with a protein biopolymer and a fluoropolymer is expected to broaden the applicability of protein-based materials.

Variation in Protein Intake Induces Variation in Spider Silk Expression

Science.gov (United States)

Blamires, Sean J.; Wu, Chun-Lin; Tso, I-Min

2012-01-01

Background It is energetically expensive to synthesize certain amino acids. The proteins (spidroins) of spider major ampullate (MA) silk, MaSp1 and MaSp2, differ in amino acid composition. Glutamine and proline are prevalent in MaSp2 and are expensive to synthesize. Since most orb web spiders express high proline silk they might preferentially attain the amino acids needed for silk from food and shift toward expressing more MaSp1 in their MA silk when starved. Methodology/Principal Findings We fed three spiders; Argiope aetherea, Cyrtophora moluccensis and Leucauge blanda, high protein, low protein or no protein solutions. A. aetherea and L. blanda MA silks are high in proline, while C. moluccesnsis MA silks are low in proline. After 10 days of feeding we determined the amino acid compositions and mechanical properties of each species' MA silk and compared them between species and treatments with pre-treatment samples, accounting for ancestry. We found that the proline and glutamine of A. aetherea and L. blanda silks were affected by protein intake; significantly decreasing under the low and no protein intake treatments. Glutmaine composition in C. moluccensis silk was likewise affected by protein intake. However, the composition of proline in their MA silk was not significantly affected by protein intake. Conclusions Our results suggest that protein limitation induces a shift toward different silk proteins with lower glutamine and/or proline content. Contradictions to the MaSp model lie in the findings that C. moluccensis MA silks did not experience a significant reduction in proline and A. aetherea did not experience a significant reduction in serine on low/no protein. The mechanical properties of the silks could not be explained by a MaSp1 expressional shift. Factors other than MaSp expression, such as the expression of spidroin-like orthologues, may impact on silk amino acid composition and spinning and glandular processes may impact mechanics. PMID:22363691

The synthesis of hydrogels with controlled distribution of polymer brushes in hydrogel network

Energy Technology Data Exchange (ETDEWEB)

Sun, YuWei; Zhou, Chao; Zhang, AoKai; Xu, LiQun; Yao, Fang [School of Chemistry and Chemical Engineering, Southeast University, Jiangning District, Nanjing, Jiangsu Province, 211189 (China); Cen, Lian, E-mail: cenlian@hotmail.com [National Tissue Engineering Center of China, No.68, East Jiang Chuan Road, Shanghai, 200241 (China); School of Chemical Engineering, East China University of Science and Technology, No.130, Mei Long Road, Shanghai, 200237 (China); Fu, Guo-Dong, E-mail: fu7352@seu.edu.cn [School of Chemistry and Chemical Engineering, Southeast University, Jiangning District, Nanjing, Jiangsu Province, 211189 (China)

2014-11-30

Highlights: • Many biological tissues are 3-dimensionally asymmetric in structure and properties, it would be desirable if hydrogels could bear such structural similarity with specialized surface and bulk properties. Moreover, gradual but continuous variation in spatial structural and property is also a common phenomenon in biological tissues, such as interfaces between bone and tendon, or between bone and cartilage. Hence, the development of a method to introduce well-defined functional polymer brushes on PEG hydrogels, especially with precisely controlled spatial structure in 3-dimensions, would impart the hydrogels with special functionalities and wider applications. Poly(ethylene glycol) (PEG) hydrogels with 3-dimensionally controlled well-defined poly(N-isopropylacrylamide) (poly(NIPAAm)) brushes were prepared by combined copper(I)-catalyzed azide-alkyne cycloaddition (“Click Chemistry”) and atom transfer radical polymerization (ATRP). The resulting hydrogels were presented as representatives with their detailed synthesis routes and characterization. H{sub PEG}-S-poly(NIPAAm) is a hydrogel with poly(NIPAAm) brushes mainly grafted on surface, whereas H{sub PEG}-G-poly(NIPAAm) has a gradiently decreased poly(NIPAAm) brushes in their chain length from surface to inside. On the other hand, poly(NIPAAm) brushes in H{sub PEG}-U-poly(NIPAAm) are uniformly dispersed throughout the whole hydrogel network. Successful preparation of H{sub PEG}-S-poly(NIPAAm), H{sub PEG}-G-poly(NIPAAm) and H{sub PEG}-U-poly(NIPAAm) were ascertained by X-ray photoelectron spectroscopy (XPS) and water contact angle measurement. Hence, the flexibility and controllability of the synthetic strategy in varying the distribution of polymer brushes and hydrogel surface properties was demonstrated. Hydrogels with tunable and well-defined 3-dimensional poly(NIPAAm) polymer brushes could be tailor-designed to find potential applications in smart devices or skin dressing, such as for diabetics

Effect of degumming ph value on electrospining of silk fibroin

Directory of Open Access Journals (Sweden)

Lu Shen-Zhou

2014-01-01

Full Text Available Regenerated silk fibroin fibers show properties dependent on the molecular weight of fibroin. The cocoon-degumming approaches had great impact on the degradation of silk fibroin. The effect of degumming pH value to electrospining of fibroin was studied in this paper. The viscosity and molecular weight of regenerated silk fibroin were studied using rheometer and gel electrophoresis. The results showed that the weaker the alkalinity of degumming reagent, there was the milder the effect on silk fibroin molecular. The fibroin fibers can be prepared by electrospining with low concentration of regenerated silk fibroin solution.

Novel β-TCP/PVA bilayered hydrogels with considerable physical and bio-functional properties for osteochondral repair.

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Yao, Hang; Kang, Junpei; Li, Weichang; Liu, Jian; Xie, Renjian; Wang, Yingjun; Liu, Sa; Wang, Dong-An; Ren, Li

2017-12-07

Cartilage repairing grafts have been widely studied, and osteochondral replacement hydrogels have proven to be an excellent method in research and clinical fields. However, it has been difficult to simultaneously solve three main issues in osteochondral replacement preparation: surface lubrication, overall mechanical support and good simulations of cell regeneration. A novel integrated bilayered hydrogel osteochondral replacement was constructed by blending polyvinyl alcohol (PVA) and β-tricalcium phosphate (β-TCP) in this study. Separated nano-ball milling with ultrasound dispersion prepared β-TCP demonstrated suitable properties of tiny particle size, high purity and ideal distribution, improving the mechanical properties of the novel integrated hydrogel, and providing a cartilage-like lubrication effect and high biocompatibility, including cytocompatibility and osteogenesis. The reinforcement of β-TCP and integrated molding technology enabled the hydrogel to demonstrate excellent component compatibility and good bonding between the two layers, which promoted the strengthening of the compression modulus and tensile modulus up to three times by mechanical testing. The surface lubrication properties of the novel osteochondral hydrogel were similar to the natural cartilage by friction coefficient characterization. The two layers of the novel integrated graft provided a considerable bio-function by co-culturing with chondrocytes and synovium mesenchymal stem cells: chondrocytes promoted adherence achieved by the upper density layer and better osteogenesis performance of the porous lower layer. The design of the bilayered β-TCP/PVA osteochondral hydrogel is promising for use in articular cartilage repair.

Fabrication of keratin-silica hydrogel for biomedical applications

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Kakkar, Prachi; Madhan, Balaraman, E-mail: bmadhan76@yahoo.co.in

2016-09-01

In the recent past, keratin has been fabricated into different forms of biomaterials like scaffold, gel, sponge, film etc. In lieu of the myriad advantages of the hydrogels for biomedical applications, a keratin-silica hydrogel was fabricated using tetraethyl orthosilicate (TEOS). Textural analysis shed light on the physical properties of the fabricated hydrogel, inturn enabling the optimization of the hydrogel. The optimized keratin-silica hydrogel was found to exhibit instant springiness, optimum hardness, with ease of spreadability. Moreover, the hydrogel showed excellent swelling with highly porous microarchitecture. MTT assay and DAPI staining revealed that keratin-silica hydrogel was biocompatible with fibroblast cells. Collectively, these properties make the fabricated keratin-silica hydrogel, a suitable dressing material for biomedical applications. - Highlights: • Keratin-silica hydrogel has been fabricated using sol–gel technique. • The hydrogel shows appropriate textural properties. • The hydrogel promotes fibroblast cells proliferation. • The hydrogel has potential soft tissue engineering applications like wound healing.

Biomolecule-Responsive Hydrogels in Medicine.

Science.gov (United States)

Sharifzadeh, Ghorbanali; Hosseinkhani, Hossein

2017-12-01

Recent advances and applications of biomolecule-responsive hydrogels, namely, glucose-responsive hydrogels, protein-responsive hydrogels, and nucleic-acid-responsive hydrogels are highlighted. However, achieving the ultimate purpose of using biomolecule-responsive hydrogels in preclinical and clinical areas is still at the very early stage and calls for more novel designing concepts and advance ideas. On the way toward the real/clinical application of biomolecule-responsive hydrogels, plenty of factors should be extensively studied and examined under both in vitro and in vivo conditions. For example, biocompatibility, biointegration, and toxicity of biomolecule-responsive hydrogels should be carefully evaluated. From the living body's point of view, biocompatibility is seriously depended on the interactions at the tissue/polymer interface. These interactions are influenced by physical nature, chemical structure, surface properties, and degradation of the materials. In addition, the developments of advanced hydrogels with tunable biological and mechanical properties which cause no/low side effects are of great importance. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Structure to function: Spider silk and human collagen

Science.gov (United States)

Rabotyagova, Olena S.

Nature has the ability to assemble a variety of simple molecules into complex functional structures with diverse properties. Collagens, silks and muscles fibers are some examples of fibrous proteins with self-assembling properties. One of the great challenges facing Science is to mimic these designs in Nature to find a way to construct molecules that are capable of organizing into functional supra-structures by self-assembly. In order to do so, a construction kit consisting of molecular building blocks along with a complete understanding on how to form functional materials is required. In this current research, the focus is on spider silk and collagen as fibrous protein-based biopolymers that can shed light on how to generate nanostructures through the complex process of self-assembly. Spider silk in fiber form offers a unique combination of high elasticity, toughness, and mechanical strength, along with biological compatibility and biodegrability. Spider silk is an example of a natural block copolymer, in which hydrophobic and hydrophilic blocks are linked together generating polymers that organize into functional materials with extraordinary properties. Since silks resemble synthetic block copolymer systems, we adopted the principles of block copolymer design from the synthetic polymer literature to build block copolymers based on spider silk sequences. Moreover, we consider spider silk to be an important model with which to study the relationships between structure and properties in our system. Thus, the first part of this work was dedicated to a novel family of spider silk block copolymers, where we generated a new family of functional spider silk-like block copolymers through recombinant DNA technology. To provide fundamental insight into relationships between peptide primary sequence, block composition, and block length and observed morphological and structural features, we used these bioengineered spider silk block copolymers to study secondary structure

Multifunctional Hydrogel with Good Structure Integrity, Self-Healing, and Tissue-Adhesive Property Formed by Combining Diels-Alder Click Reaction and Acylhydrazone Bond.

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Yu, Feng; Cao, Xiaodong; Du, Jie; Wang, Gang; Chen, Xiaofeng

2015-11-04

Hydrogel, as a good cartilage tissue-engineered scaffold, not only has to possess robust mechanical property but also has to have an intrinsic self-healing property to integrate itself or the surrounding host cartilage. In this work a double cross-linked network (DN) was designed and prepared by combining Diels-Alder click reaction and acylhydrazone bond. The DA reaction maintained the hydrogel's structural integrity and mechanical strength in physiological environment, while the dynamic covalent acylhydrazone bond resulted in hydrogel's self-healing property and controlled the on-off switch of network cross-link density. At the same time, the aldehyde groups contained in hydrogel further promote good integration of the hydrogel to surrounding tissue based on aldehyde-amine Schiff-base reaction. This kind of hydrogel has good structural integrity, autonomous self-healing, and tissue-adhesive property and simultaneously will have a good application in tissue engineering and tissue repair field.

Silk sericin/polyacrylamide in situ forming hydrogels for dermal reconstruction.

Science.gov (United States)

Kundu, Banani; Kundu, Subhas C

2012-10-01

In situ forming tissue sealants are advantageous due to ease in application, complete coverage of defect site and assured comfort levels to patients. The interconnected three-dimensional hydrophilic networks perfectly manage typical dermal wounds by suitably scaffolding skin fibroblast, diffusing the nutrients, therapeutics and exudates while still maintaining an adequately moist environment. We evaluate the cell homing ability of semi-interpenetrating non-mulberry tropical tasar silk sericin/polyacrylamide hydrophilic network with a keen understanding of its network characteristics and correlation of protein concentration with the performance as cell scaffold. Interconnectivity of porous networks observed through scanning electron micrograph revealed pore sizes ranging from 23 to 52 μm. The enhanced β-sheet content with the increasing sericin concentration in far red spectroscopy study supported their corresponding improved compressive strength. These semi-interpenetrating networks were found to possess a maximum fluid uptake of 112% of its weight, hence preventing the accumulation of exudates at the wound area. The present systems appear to possess characteristics like rapid gelation (~5min) at 37 °C, 98% porosity enabling the migration of fibroblasts during healing (observed through confocal and scanning electron micrographs), cell adhesion together with the absence of any cyto-toxic effect suggesting its potential as in situ tissue sealants. The compressive strength up to 61 kPa ensured ease in handling even when wet. The results prove the suitability to use non-mulberry tasar cocoon silk sericin/polyacrylamide semi-interpenetrating network as a reconstructive dermal sealant. Copyright © 2012 Elsevier Ltd. All rights reserved.

Reinforcing the inner phase of the filled hydrogels with CNTs alters drug release properties and human keratinocyte morphology: A study on the gelatin- tamarind gum filled hydrogels.

Science.gov (United States)

Maharana, Vivek; Gaur, Deepanjali; Nayak, Suraj K; Singh, Vinay K; Chakraborty, Subhabrata; Banerjee, Indranil; Ray, Sirsendu S; Anis, Arfat; Pal, Kunal

2017-11-01

The study reports the synthesis and characterization of gelatin-tamarind gum (TG) based filled hydrogels for drug delivery applications. In this study, three different types of carbon nanotubes (CNTs) were incorporated within the dispersed TG phase of the filled hydrogels. The prepared hydrogels were thoroughly characterised using bright field microscope, FESEM, FTIR spectroscopy, differential scanning calorimeter, and mechanical tester. The swelling and the drug (salicylic acid) release properties of the filled hydrogels were also evaluated. The micrographs revealed the formation of biphasic systems. The internal phase appeared as agglomerates, and the CNTs were confined within the dispersed TG phase. FTIR and XRD studies revealed that CNTs promoted associative interactions among the components of the hydrogel, which promoted the formation of large crystallite size. The mechanical study indicated better resistance to the breakdown of the architecture of the CNT-containing filled hydrogels. Drug release studies, both passive and iontophoretic, suggested that the non-Fickian diffusion of the drug was prevalent during its release from hydrogel matrices. The prepared hydrogels were cytocompatible with human keratinocytes. The results suggested the probable use of such hydrogels in wound healing, tissue engineering and drug delivery applications. Copyright © 2017 Elsevier Ltd. All rights reserved.

Studies on the properties of poly(ethylene oxide) R-150 water-swollen hydrogel formed by irradiation

International Nuclear Information System (INIS)

Yang Zhanshan; Zhu Nankang; Yang Shuqin; Qiang Yizhong

2000-01-01

The physical and chemical properties of PEO R-150 water-swollen hydrogel films formed by electron beam irradiation are studied and compared with PEO R-150 hydrogel films. The experimental results show that the irradiation dose and mass fraction of the polymer do not produce a significant effect on the gel fraction, of the PEO R-150 water-swollen hydrogel films (P>0.05). The degrees of swelling of the PEO R-150 water-swollen hydrogel films decrease as the irradiation dose increasing (P 0.05). The results indicate that the saturant crosslinking density, the lowest degree of swelling of the PEO R-150 water-swollen hydrogel films produce and unfavorable effect on their machinery strength

Enhanced Mechanical Properties in Cellulose Nanocrystal-Poly(oligoethylene glycol methacrylate) Injectable Nanocomposite Hydrogels through Control of Physical and Chemical Cross-Linking.

Science.gov (United States)

De France, Kevin J; Chan, Katelyn J W; Cranston, Emily D; Hoare, Todd

2016-02-08

While injectable hydrogels have several advantages in the context of biomedical use, their generally weak mechanical properties often limit their applications. Herein, we describe in situ-gelling nanocomposite hydrogels based on poly(oligoethylene glycol methacrylate) (POEGMA) and rigid rod-like cellulose nanocrystals (CNCs) that can overcome this challenge. By physically incorporating CNCs into hydrazone cross-linked POEGMA hydrogels, macroscopic properties including gelation rate, swelling kinetics, mechanical properties, and hydrogel stability can be readily tailored. Strong adsorption of aldehyde- and hydrazide-modified POEGMA precursor polymers onto the surface of CNCs promotes uniform dispersion of CNCs within the hydrogel, imparts physical cross-links throughout the network, and significantly improves mechanical strength overall, as demonstrated by quartz crystal microbalance gravimetry and rheometry. When POEGMA hydrogels containing mixtures of long and short ethylene oxide side chain precursor polymers were prepared, transmission electron microscopy reveals that phase segregation occurs with CNCs hypothesized to preferentially locate within the stronger adsorbing short side chain polymer domains. Incorporating as little as 5 wt % CNCs results in dramatic enhancements in mechanical properties (up to 35-fold increases in storage modulus) coupled with faster gelation rates, decreased swelling ratios, and increased stability versus hydrolysis. Furthermore, cell viability can be maintained within 3D culture using these hydrogels independent of the CNC content. These properties collectively make POEGMA-CNC nanocomposite hydrogels of potential interest for various biomedical applications including tissue engineering scaffolds for stiffer tissues or platforms for cell growth.

Antibacterial Properties of Silver Nanoparticles Embedded on Polyelectrolyte Hydrogels Based on α-Amino Acid Residues

Directory of Open Access Journals (Sweden)

Mario Casolaro

2018-05-01

Full Text Available Polyelectrolyte hydrogels bearing l-phenylalanine (PHE, l-valine (AVA, and l-histidine (Hist residues were used as scaffolds for the formation of silver nanoparticles by reduction of Ag+ ions with NaBH4. The interaction with the metal ion allowed a prompt collapse of the swollen hydrogel, due to the neutralization reaction of basic groups present on the polymer. The imidazole nitrogen of the hydrogel with Hist demonstrated greater complexing capacity with the Ag+ ion compared to the hydrogels with carboxyl groups. The subsequent reduction to metallic silver allowed for the restoration of the hydrogel’s degree of swelling to the starting value. Transmission electron microscopy (TEM and spectroscopic analyses showed, respectively, a uniform distribution of the 15 nm spherical silver nanoparticles embedded on the hydrogel and peak optical properties around a wavelength of 400 nm due to the surface plasmonic effect. Unlike native hydrogels, the composite hydrogels containing silver nanoparticles showed good antibacterial activity as gram+/gram− bactericides, and higher antifungal activity against S. cerevisiae.

Preparation and physico-chemical properties of hydrogels from carboxymethyl cassava starch crosslinked with citric acid

Science.gov (United States)

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.

Electrochemical characterization of hydrogels for biomimetic applications

DEFF Research Database (Denmark)

Peláez, L.; Romero, V.; Escalera, S.

2011-01-01

) or a photoinitiator (P) to encapsulate and stabilize biomimetic membranes for novel separation technologies or biosensor applications. In this paper, we have investigated the electrochemical properties of the hydrogels used for membrane encapsulation. Specifically, we studied the crosslinked hydrogels by using...... electrochemical impedance spectroscopy (EIS), and we demonstrated that chemically crosslinked hydrogels had lower values for the effective electrical resistance and higher values for the electrical capacitance compared with hydrogels with photoinitiated crosslinking. Transport numbers were obtained using......〉 and 〈Pw〉 values than PEG‐1000‐DMA‐P and PEG‐400‐DA‐P hydrogels. In conclusion, our results show that hydrogel electrochemical properties can be controlled by the choice of polymer and type of crosslinking used and that their water and salt permeability properties are congruent with the use of hydrogels...

Influence of natural and synthetic crosslinking reagents on the structural and mechanical properties of chitosan-based hybrid hydrogels.

Science.gov (United States)

Garnica-Palafox, I M; Sánchez-Arévalo, F M

2016-10-20

The objective of this work was to correlate the physical and chemical properties of chitosan/poly(vinyl alcohol)/genipin (CS/PVA/GEN) and chitosan/poly(vinyl alcohol)/glutaraldehyde (CS/PVA/GA) hydrogels with their structural and mechanical responses. In addition, their molecular structures were determined and confirmed using FTIR spectroscopy. The results indicated that the hybrid hydrogels crosslinked with genipin showed similar crystallinity, thermal properties, elongation ratio and structural parameters as those crosslinked with glutaraldehyde. However, it was found that the elastic moduli of the two hybrid hydrogels were slightly different: 2.82±0.33MPa and 2.08±0.11MPa for GA and GEN, respectively. Although the hybrid hydrogels crosslinked with GEN presented a lower elastic modulus, the main advantage is that GEN is five to ten thousand times less cytotoxic than GA. This means that the structural and mechanical properties of hybrid hydrogels crosslinked with GEN can easily be tuned and could have potential applications in the tissue engineering, regenerative medicine, food, agriculture and environmental industries. Copyright © 2016 Elsevier Ltd. All rights reserved.

Functionalized bioengineered spider silk spheres improve nuclease resistance and activity of oligonucleotide therapeutics providing a strategy for cancer treatment.

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Kozlowska, Anna Karolina; Florczak, Anna; Smialek, Maciej; Dondajewska, Ewelina; Mackiewicz, Andrzej; Kortylewski, Marcin; Dams-Kozlowska, Hanna

2017-09-01

Cell-selective delivery and sensitivity to serum nucleases remain major hurdles to the clinical application of RNA-based oligonucleotide therapeutics, such as siRNA. Spider silk shows great potential as a biomaterial due to its biocompatibility and biodegradability. Self-assembling properties of silk proteins allow for processing into several different morphologies such as fibers, scaffolds, films, hydrogels, capsules and spheres. Moreover, bioengineering of spider silk protein sequences can functionalize silk by adding peptide moieties with specific features including binding or cell recognition domains. We demonstrated that modification of silk protein by adding the nucleic acid binding domain enabled the development of a novel oligonucleotide delivery system that can be utilized to improve pharmacokinetics of RNA-based therapeutics, such as CpG-siRNA. The MS2 bioengineered silk was functionalized with poly-lysine domain (KN) to generate hybrid silk MS2KN. CpG-siRNA efficiently bound to MS2KN in contrary to control MS2. Both MS2KN complexes and spheres protected CpG-siRNA from degradation by serum nucleases. CpG-siRNA molecules encapsulated into MS2KN spheres were efficiently internalized and processed by TLR9-positive macrophages. Importantly, CpG-STAT3siRNA loaded in silk spheres showed delayed and extended target gene silencing compared to naked oligonucleotides. The prolonged Stat3 silencing resulted in the more pronounced downregulation of interleukin 6 (IL-6), a proinflammatory cytokine and upstream activator of STAT3, which limits the efficacy of TLR9 immunostimulation. Our results demonstrate the feasibility of using spider silk spheres as a carrier of therapeutic nucleic acids. Moreover, the modified kinetic and activity of the CpG-STAT3siRNA embedded into silk spheres is likely to improve immunotherapeutic effects in vivo. We demonstrated that modification of silk protein by adding the nucleic acid binding domain enabled the development of a novel

Silk film biomaterials for ocular surface repair

Science.gov (United States)

Lawrence, Brian David

Current biomaterial approaches for repairing the cornea's ocular surface upon injury are partially effective due to inherent material limitations. As a result there is a need to expand the biomaterial options available for use in the eye, which in turn will help to expand new clinical innovations and technology development. The studies illustrated here are a collection of work to further characterize silk film biomaterials for use on the ocular surface. Silk films were produced from regenerated fibroin protein solution derived from the Bombyx mori silkworm cocoon. Methods of silk film processing and production were developed to produce consistent biomaterials for in vitro and in vivo evaluation. A wide range of experiments was undertaken that spanned from in vitro silk film material characterization to in vivo evaluation. It was found that a variety of silk film properties could be controlled through a water-annealing process. Silk films were then generated that could be use in vitro to produce stratified corneal epithelial cell sheets comparable to tissue grown on the clinical standard substrate of amniotic membrane. This understanding was translated to produce a silk film design that enhanced corneal healing in vivo on a rabbit injury model. Further work produced silk films with varying surface topographies that were used as a simplified analog to the corneal basement membrane surface in vitro. These studies demonstrated that silk film surface topography is capable of directing corneal epithelial cell attachment, growth, and migration response. Most notably epithelial tissue development was controllably directed by the presence of the silk surface topography through increasing cell sheet migration efficiency at the individual cellular level. Taken together, the presented findings represent a comprehensive characterization of silk film biomaterials for use in ocular surface reconstruction, and indicate their utility as a potential material choice in the

Surface and anti-fouling properties of a polyampholyte hydrogel grafted onto a polyethersulfone membrane.

Science.gov (United States)

Zhang, Wei; Yang, Zhe; Kaufman, Yair; Bernstein, Roy

2018-05-01

Zwitterion polymers have anti-fouling properties; therefore, grafting new zwitterions to surfaces, particularly as hydrogels, is one of the leading research directions for preventing fouling. Specifically, polyampholytes, polymers of random mixed charged subunits with a net-electric charge, offer a synthetically easy alternative for studying new zwitterions with a broad spectrum of charged moieties. Here, a novel polyampholyte hydrogel was grafted onto the surface of polyethersulfone membrane by copolymerizing a mixture of vinylsulfonic acid (VSA) and [2-(methacryloyloxy)ethyl]trimethylammonium chloride (METMAC) as the negatively and positively charged monomers, respectively, using various monomer ratios in the polymerization solution, and with N,N'-methylenebisacrylamide as the crosslinker. The physicochemical, morphological and anti-fouling properties of the modified membranes were systematically investigated. Hydrophilic hydrogels were successfully grafted using monomers at different molar ratios. A thin-film zwitterion hydrogel (∼90 nm) was achieved at a 3:1 [VSA:METMAC] molar ratio in the polymerization solution. Among all examined membranes, the zwitterion polyampholyte-modified membrane demonstrated the lowest adsorption of proteins, humic acid, and sodium alginate. It also had low fouling and high flux recovery following filtration with a protein or with an extracellular polymeric substance solution. These findings suggest that this polyampholyte hydrogel is applicable as a low fouling surface coating. Copyright © 2018 Elsevier Inc. All rights reserved.

The influence of water quality on properties of hydrogel membranes prepared by ionizing radiation

International Nuclear Information System (INIS)

Alcantara, Mara Tania S.; Sisti, Cristina; Furusawa, Helio A.; Lugao, Ademar B.

2009-01-01

Insoluble hydrogels are crosslinked polymeric materials which have ability to absorb significant amounts of water in their three-dimensional polymeric matrix. Ionizing radiation has been used in hydrogels preparation allowing the structure formation and sterilization simultaneously in only one step without necessity to add any initiators crosslinkers. These advantages make irradiation an useful method for synthesis of hydrogels, especially for biomedical use. There are numerous applications of hydrogels such as contact lenses, drug delivery devices, wound dressings, etc. Poly(N-vinyl-2-pyrrolidone) (PVP) is a water soluble polymer, which exhibits a series of interactions in aqueous solutions. The aim of this work is to investigate the effect of ions present in distillated water to prepare PVP hydrogels because Hofmeister series ions have the capacity to change the water structure that represents the largest fraction of the system. Another reason is that the use of high purity water can be costly in large industrial production of these materials. Hydrogels with 12% and 20% of PVP were prepared using distillated and ultrapure water. The polymerization was induced by gamma radiation at 25 kGy. For the investigation of the distillated water effect, the ions present as impurities were identified by ion chromatography. Physical-chemical properties such as degree of crosslinking of hydrogels was determined using gel fraction methodology and swelling kinetic was studied in the prepared hydrogels. (author)

Silk fibroin/gold nanocrystals: a new example of biopolymer-based nanocomposites

Science.gov (United States)

Noinville, S.; Garnier, A.; Courty, A.

2017-05-01

The dispersion of nanoparticles in ordered polymer nanostructures can provide control over particle location and orientation, and pave the way for tailored nanomaterials that have enhanced mechanical, electrical, or optical properties. Here we used silk fibroin, a natural biopolymer, to embed gold nanocrystals (NCs), so as to obtain well-ordered structures such as nanowires and self-assembled triangular nanocomposites. Monodisperse gold NCs synthesized in organic media are mixed to silk fibroin and the obtained nanocomposites are characterized by UV-visible spectroscopy, transmission electron microscopy (TEM), scanning electron microscopy (FE-SEM), atomic force microscopy (AFM) and Infrared spectroscopy. The optical properties study of gold NCs and silk-gold nanocomposites shows that the Surface Plasmon band is blue shifted compared to gold NCs. The size and shape of NCs gold superlattices can be well controlled by the presence of silk fibroin giving nanowires and also self-assembled triangular nanocomposites as characterized by TEM, FE-SEM and AFM. The strong interaction between gold NCs and silk fibroin is also revealed by the conformation change of silk protein in presence of gold NCs, as shown by FTIR analysis. The formation of such ordered nanocomposites (gold NCs/silk fibroin) will provide new nanoplasmonic devices.

Structural analysis and application to biomaterials of the silk fibroins

International Nuclear Information System (INIS)

Nakazawa, Yasumoto

2010-01-01

Silk fibroin from Bombyx mori silkworm has outstanding mechanical properties despite being spun from aqueous solution. I have clarified two distinct structures in the solid state; silk I and silk II, which mean the structures before and after spinning, by using solid state NMR. Moreover, I have been developing several kinds of biomaterials, such as bone regeneration materials and vascular grafts. In this paper, I present two topics: one is the structural analyses of the silk fibroin in detail, the other is applications of silk fibroins to tissue engineering. In the case of vascular regeneration, I have developed the small diameter vascular grafts made by silk fibroins. The new grafts from silk fibroins have good patency, and these grafts were commonly covered with cells and platelets at 4 weeks after implantation. For bone tissue engineering, I performed structural analyses of a new silk-like peptide, E n (AGSGAG) 4 , in order to consider the molecular design of biomaterials for bone regeneration. (author)

Spider-silk-like shape memory polymer fiber for vibration damping

International Nuclear Information System (INIS)

Yang, Qianxi; Li, Guoqiang

2014-01-01

In this study, the static and dynamic properties of shape memory polyurethane (SMPU) fiber are reported and compared to those of spider dragline silk. Although the polymeric fiber has a lower strength compared to spider dragline silks (0.2–0.3 GPa versus 1.1 GPa), it possesses much higher toughness (276–289 MJ m −3 versus 160 MJ m −3 ), due to its excellent extensibility. The dynamic mechanical tests reveal that SMPU fiber has a high damping capacity (tan δ = 0.10–0.35) which is comparable to or even higher than that of spider silks (tan δ = 0.15). In addition, we found that, different programming methods change the shape memory and damping properties of the fiber in different ways and cold-drawing programming is more advocated in structural applications. These results suggest that the SMPU fiber has similar vibration damping and mechanical properties as spider silk, and may find applications in lightweight engineering structures. (paper)

Swelling and mechanical properties of physically crosslinked poly(vinyl alcohol) hydrogels.

Science.gov (United States)

Suzuki, Atsushi; Sasaki, Saori

2015-12-01

Physically crosslinked poly(vinyl alcohol) gels are versatile biomaterials due to their excellent biocompatibility. In the past decades, physically crosslinked poly(vinyl alcohol) and poly(vinyl alcohol)-based hydrogels have been extensively studied for biomedical applications. However, these materials have not yet been implemented due to their mechanical strength. Physically crosslinked poly(vinyl alcohol) gels consist of a swollen amorphous network of poly(vinyl alcohol) physically crosslinked by microcrystallites. Although the mechanical properties can be improved to some extent by controlling the distribution of microcrystallites on the nano- and micro-scales, enhancing the mechanical properties while maintaining high water content remains very difficult. It may be technologically impossible to significantly improve the mechanical properties while keeping the gel's high water absorbance ability using conventional fabrication methods. Physical and chemical understandings of the swelling and mechanical properties of physically crosslinked poly(vinyl alcohol) gels are considered here; some promising strategies for their practical applications are presented. This review focuses more on the recent studies on swelling and mechanical properties of poly(vinyl alcohol) hydrogels, prepared using only poly(vinyl alcohol) and pure water with no other chemicals, as potential biomedical materials. © IMechE 2015.

Radiation-induced synthesis and swelling properties of p(2-hydroxyethyl methacrylate/itaconic acid/oligo (ethylene glycol) acrylate) terpolymeric hydrogels

International Nuclear Information System (INIS)

Micic, M.; Stamenic, D.; Suljovrujic, E.

2012-01-01

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. - Highlights: ► pH- and thermo-sensitive P(HEMA/IA/OEGA) hydrogels were synthesised by γ radiation. ► OEGA units have a large hydrophilic potential. ► Swelling capacity increases with the OEGA content. ► Variation in composition of hydrogels can give

Coating of Silk Fabric Using PVA/Ciprofloxacin Hcl Nanofibers for Biomedical Applications

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Somaye Baghersad

2016-05-01

Full Text Available In recent years, fabrication of polymeric antibacterial wound dressing has gained most attention in controlling wound infections. Silk is also a member of the broad family of protein-based polmers. The silk produced by the lepidopteran insect Bombyx mori is a highly accepted material due to its long history as a very valuable textile fiber. Recently, additional applications have been developed for silk, mainly in the field of biotechnology. Regarding its importance in wound healing, silk fabric was incorporated with ciprofloxacin, as an antibiotic, on its surface coated with electro-spun PVA/ciprofloxacin nanofibers. Before coating, degumming was carried out using autoclave technique and properties of the silk fabric, before and after degumming process, was investigated by SEM, FTIR, mechanical properties and moisture absorbance measurement. The results of all analyses showed a reduction in fibers diameter, mechanical strength and moisture absorption after degumming process. Electrospinning condition was optimized and diameter of the nanofibers, with and without drug, was measured before coating. The results showed that addition of the drug increased electrical conductivity of electrospinning solution and resulted in finer nanofibers. Antibacterial test was performed using "disk diffusion method" with Escherichia coli (EC and Staphylococcus aureus (SA bacteria to compare the antibacterial properties of degummed and non-degummed silk fabrics alone and coated with nanofibers. Measurement of bacterial inhibition zone diameter showed no antibacterial activity for degummed and non-degummed silk fabrics alone. However, the sample coated with PVA/ciprofloxacin showed antibacterial activity. The antibacterial property for SA in both cases was the same, but for EC, the antibacterial activity of degummed silk fabric was more than that of non-degummed material.

The osteogenic potential of mesoporous bioglasses/silk and non-mesoporous bioglasses/silk scaffolds in ovariectomized rats: in vitro and in vivo evaluation.

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Ning Cheng

Full Text Available Silk-based scaffolds have been introduced to bone tissue regeneration for years, however, their local therapeutic efficiency in bone metabolic disease condition has been seldom reported. According to our previous report, mesoporous bioactive glass (MBG/silk scaffolds exhibits superior in vitro bioactivity and in vivo osteogenic properties compared to non-mesoporous bioactive glass (BG/silk scaffolds, but no information could be found about their efficiency in osteoporotic (OVX environment. This study investigated a biomaterial-based approach for improving MSCs behavior in vitro, and accelerating OVX defect healing by using 3D BG/silk and MBG/silk scaffolds, and pure silk scaffolds as control. The results of SEM, CCK-8 assay and quantitative ALP activity showed that MBG/silk scaffolds can improve attachment, proliferation and osteogenic differentiation of both O-MSCs and sham control. In vivo therapeutic efficiency was evaluated by μCT analysis, hematoxylin and eosin staining, safranin O staining and tartrate-resistant acid phosphatase, indicating accelerated bone formation with compatible scaffold degradation and reduced osteoclastic response of defect healing in OVX rats after 2 and 4 weeks treatment, with a rank order of MBG/silk > BG/silk > silk group. Immunohistochemical markers of COL I, OPN, BSP and OCN also revealed that MBG/silk scaffolds can better induce accelerated collagen and non-collagen matrix production. The findings of this study suggest that MBG/silk scaffolds provide a better environment for cell attachment, proliferation and differentiation, and act as potential substitute for treating local osteoporotic defects.

Structural study of Bombyx mori silk fibroin during processing for regeneration

Science.gov (United States)

Ha, Sung-Won

Bombyx mori silk fibroin has excellent mechanical properties combined with flexibility, tissue compatibility, and high oxygen permeability in the wet condition. This important material should be dissolved and regenerated to be utilized as useful forms such as gel, film, fiber, powder, or non-woven. However, it has long been a problem that the regenerated fibroin materials show poor mechanical properties and brittleness. These problems were technically solved by improving a fiber processing method reported here. The regenerated fibroin fibers showed much better mechanical properties compared to the original silk fibers. This improved technique for the fiber processing of Bombyx mori silk fibroin may be used as a model system for other semi-crystalline fiber forming proteins, becoming available through biotechnology. The physical and chemical properties of the regenerated fibers were characterized by SinTechRTM tensile testing, X-ray diffraction, solid state 13C NMR spectroscopy, and SEM. Unlike synthetic polymers, the molecular weight distribution of Bombyx mori silk fibroin is mono-disperse because silk fibroin is synthesized from DNA template. Genetic studies have revealed the entire amino acid sequence of Bombyx mori silk fibroin. It is known that the crystalline silk II structure is composed of hexa-amino acid sequences, GAGAGS. However, in the amino acid sequence of Bombyx mori silk fibroin heavy chain, there are present 11 chemically irregular but evolutionarily conserved sequences with about 31 amino acid residues (irregular GT˜GT sequences). The structure and role of these irregular sequences have remained unknown. One of the most frequently appearing irregular sequences was synthesized by a peptide synthesizer. The three-dimensional structure of this irregular silk peptide was studied by the high resolution two-dimensional NMR technique. The three-dimensional structure of this peptide shows that it makes a turn or loop structure (distorted O shape), which

Poly(amido-amine)-based hydrogels with tailored mechanical properties and degradation rates for tissue engineering.

Science.gov (United States)

Martello, Federico; Tocchio, Alessandro; Tamplenizza, Margherita; Gerges, Irini; Pistis, Valentina; Recenti, Rossella; Bortolin, Monica; Del Fabbro, Massimo; Argentiere, Simona; Milani, Paolo; Lenardi, Cristina

2014-03-01

Poly(amido-amine) (PAA) hydrogels containing the 2,2-bisacrylamidoacetic acid-4-amminobutyl guanidine monomeric unit have a known ability to enhance cellular adhesion by interacting with the arginin-glycin-aspartic acid (RGD)-binding αVβ3 integrin, expressed by a wide number of cell types. Scientific interest in this class of materials has traditionally been hampered by their poor mechanical properties and restricted range of degradation rate. Here we present the design of novel biocompatible, RGD-mimic PAA-based hydrogels with wide and tunable degradation rates as well as improved mechanical and biological properties for biomedical applications. This is achieved by radical polymerization of acrylamide-terminated PAA oligomers in both the presence and absence of 2-hydroxyethylmethacrylate. The degradation rate is found to be precisely tunable by adjusting the PAA oligomer molecular weight and acrylic co-monomer concentration in the starting reaction mixture. Cell adhesion and proliferation tests on Madin-Darby canine kidney epithelial cells show that PAA-based hydrogels have the capacity to promote cell adhesion up to 200% compared to the control. Mechanical tests show higher compressive strength of acrylic chain containing hydrogels compared to traditional PAA hydrogels. Copyright © 2013 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Mechanical properties of poly(N-isopropylacrylamide-Co-itaconic acid) hydrogels

International Nuclear Information System (INIS)

Valderruten, N. E.; Quintana, J. R.; Katime, I.

2001-01-01

It is well known that polymers of N-isopropylacrylamide (NIPA) show lower critical solution temperature (LCST) behavior in water and its gels have a volume phase transition at about 34 degree centigree in water. In this study, we reported the polymerization of NIPA in the presence of N,N methylenebisacrylamide (BIS). Poly(N-isopropylacrylamide) and poly(N-isopropylacrylamide-co-itaconic acid) hydrogels were obtained by swelling the resultant solid xerogels to equilibrium in water. The effects of monomer composition and concentration of added cross-linking agent on the swelling behavior and mechanical properties of these hydrogels at 22 and 37 degree centigree were investigated, the latter involving measurements of shear in a DMTA system. The storage moduli at 22 degree centigree lay within the range 9.08-5.08 KPa. At a fixed BIS concentration, an increase from 22 to 37 degree centigree resulted in an increase in the shear moduli and the effective crosslinking density (v e ) and a decrease in the interaction parameter hydrogel/water, χ. (Author) 6 refs

Addition of selenium nanoparticles to electrospun silk scaffolds improves mammalian cell activity while reducing bacterial growth

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Stanley Chung

2016-07-01

Full Text Available Silk possesses many beneficial wound healing properties, and electrospun scaffolds are especially applicable for skin applications, due to their smaller interstices and higher surface areas compared to non-electrospun equivalents. However, purified silk promotes microbial growth. In contrast, selenium nanoparticles have excellent antibacterial properties and are a novel antimicrobial chemistry. Here, electrospun silk scaffolds were doped with selenium nanoparticles to impart antibacterial properties to the silk scaffolds. Results showed significantly improved bacterial inhibition and improvement in human dermal fibroblast metabolic activity. These results suggest that the addition of selenium nanoparticles to electrospun silk is a promising approach to improve wound healing with reduced infection, without relying on antibiotics.

Influence of electron irradiation on the structural and thermal properties of silk fibroin films

Energy Technology Data Exchange (ETDEWEB)

Asha, S.; Sangappa,; Sanjeev, Ganesh, E-mail: ganeshanjeev@rediffmail.com [Department of Studies in Physics, Mangalore University, Mangalagangotri, Mangalore - 574 199 (India)

2015-06-24

Radiation-induced changes in Bombyx mori silk fibroin (SF) films under electron irradiation were investigated and correlated with dose. SF films were irradiated in air at room temperature using 8 MeV electron beam in the range 0-150 kGy. Various properties of the irradiated SF films were studied using X-ray diffraction (XRD), Differential Scanning Calorimetry (DSC) and Thermogravimetric Analysis (TGA). Electron irradiation was found to induce changes in the physical and thermal properties, depending on the radiation dose.

Effect of Sodium Salicylate on the Viscoelastic Properties and Stability of Polyacrylate-Based Hydrogels for Medical Applications

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Zuzana Kolarova Raskova

2016-01-01

Full Text Available Investigation was made into the effect exerted by the presence of sodium salicylate (0–2 wt.%, in Carbomer-based hydrogel systems, on processing conditions, rheological and antimicrobial properties in tests against Gram-positive (Staphylococcus aureus and Gram-negative (Escherichia coli bacterial strains, and examples of yeast (Candida albicans and mould (Aspergillus niger. In addition, the work presents an examination of long-term stability by means of aging over one year the given hydrogels at 8°C and 25°C. The results show that 0.5 wt.% NaSal demonstrated a noticeable effect on the hydrogel neutralization process, viscosity, and antimicrobial properties against all of the tested microorganisms. The long-term stability studies revealed that hydrogels can maintain antimicrobial activity as well as viscosity to a degree that would be sufficient for practical use.

The study of polymeric hydro-gels with unique properties obtained by polymerization with gamma radiation processing

International Nuclear Information System (INIS)

Dragusin, M.

1995-01-01

This thesis presents the work carried out on polymeric hydro-gels obtained by radiation processing using 60 Co gamma rays from the irradiation facility IETI-10.000 (10 k Ci), and on the polymeric hydro-gels obtained by irradiation with the electron beams from a linear accelerator (6 MeV). The aim of the study was to determine the effect of the rate dose and total dose absorbed in the materials. There are presented the preparation methods of homo- and co-polymer hydro-gels (acrylics, namely anionic and neutral monomers (acrylamide, acrylic acid, vinyl acetate) and cationic monomers (di-methyl di-allyl ammonium chloride)) such as floculants, additives, absorbers, etc. Concerning with these we have analysed the preparation methods, the mechanical, thermal, diffusivity, and swelling properties of polymeric hydro-gels in a large variety of gels of type I or II. The technological aspects and end use were studied in connection with the characteristics of the radiation processing of these hydro-gels as a function of chemical composition rate and absorbed dose, swelling degree (low and very high hydro-soluble), mechanical and diffusional properties. (author) 33 figs., 12 tabs., 101 refs

Superhydrophobic, Superoleophobic and Antimicrobial Coatings for the Protection of Silk Textiles

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Dimitra Aslanidou

2018-03-01

Full Text Available A method to produce multifunctional coatings for the protection of silk is developed. Aqueous dispersion, free of any organic solvent, containing alkoxy silanes, organic fluoropolymer, silane quaternary ammonium salt, and silica nanoparticles (7 nm in mean diameter is sprayed onto silk which obtains (i superhydrophobic and superoleophobic properties, as evidenced by the high contact angles (>150° of water and oil drops and (ii antimicrobial properties. Potato dextrose agar is used as culture medium for the growth of microorganisms. The protective coating hinders the microbial growth on coated silk which remains almost free of contamination after extensive exposure to the microorganisms. Furthermore, the multifunctional coating induces a moderate reduction in vapor permeability of the treated silk, it shows very good durability against abrasion and has a minor visual effect on the aesthetic appearance of silk. The distinctive roles of the silica nanoparticles and the antimicrobial agent on the aforementioned properties of the coating are investigated. Silica nanoparticles induce surface structures at the micro/nano-meter scale and are therefore responsible for the achieved extreme wetting properties that promote the antimicrobial activity. The latter is further enhanced by adding the silane quaternary ammonium salt in the composition of the protective coating.

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

Science.gov (United States)

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

Effect of Strongly Alkaline Electrolyzed Water on Silk Degumming and the Physical Properties of the Fibroin Fiber.

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Ting-Ting Cao

Full Text Available Strongly alkaline electrolyzed water (SAEW was prepared by electrolysis of tap water in a laboratory-made water electrolyzer. The pH of stored SAEW was stable for more than one month. The hardness of the electrolyzed water was 30% lower and the Na(+ concentration was 18% higher than those of the tap water. Silkworm cocoon shells were boiled in pH 11.50 SAEW at a ratio of 1∶40∼80 (W/V for 20 min and the sericin layers around the silk fibroin fibers were removed completely. The tensile properties and thermal decomposition temperature of a single filament of silk fibroin obtained by the SAEW method were almost the same as those for the fiber obtained by the neutral soap, and much higher than those for the fiber obtained by Na2CO3 degumming. The results demonstrate that SAEW is an environmentally friendly and pollution-free silk degumming agent that allows highly efficient, low cost recovery of sericin.

Cytocompatible cellulose hydrogels containing trace lignin

International Nuclear Information System (INIS)

Nakasone, Kazuki; Kobayashi, Takaomi

2016-01-01

Sugarcane bagasse was used as a cellulose resource to prepare transparent and flexible cellulose hydrogel films. On the purification process from bagasse to cellulose, the effect of lignin residues in the cellulose was examined for the properties and cytocompatibility of the resultant hydrogel films. The cellulose was dissolved in lithium chloride/N,N-dimethylacetamide solution and converted to hydrogel films by phase inversion. In the purification process, sodium hydroxide (NaOH) treatment time was changed from 1 to 12 h. This resulted in cellulose hydrogel films having small amounts of lignin from 1.62 to 0.68%. The remaining lignin greatly affected hydrogel properties. Water content of the hydrogel films was increased from 1153 to 1525% with a decrease of lignin content. Moreover, lower lignin content caused weakening of tensile strength from 0.80 to 0.43 N/mm"2 and elongation from 45.2 to 26.5%. Also, similar tendency was observed in viscoelastic behavior of the cellulose hydrogel films. Evidence was shown that the lignin residue was effective for the high strength of the hydrogel films. In addition, scanning probe microscopy in the morphological observation was suggested that the trace lignin in the cellulose hydrogel affected the cellulose fiber aggregation in the hydrogel network. The trace of lignin in the hydrogels also influenced fibroblast cell culture on the hydrogel films. The hydrogel film containing 1.68% lignin showed better fibroblast compatibility as compared to cell culture polystyrene dish used as reference. - Highlights: • Cellulose hydrogel films with trace lignin were obtained from sugarcane bagasse. • Lignin content was found to be in the range of 1.62 − 0.68% by UV–Vis spectroscopy. • Higher lignin content strengthened mechanical properties of the hydrogel films. • Trace lignin affected the hydrogel morphology such as roughness and porosity. • High cell proliferation was observed in the hydrogel containing 1.68% lignin.

Cytocompatible cellulose hydrogels containing trace lignin

Energy Technology Data Exchange (ETDEWEB)

Nakasone, Kazuki; Kobayashi, Takaomi, E-mail: takaomi@nagaoakut.ac.jp

2016-07-01

Sugarcane bagasse was used as a cellulose resource to prepare transparent and flexible cellulose hydrogel films. On the purification process from bagasse to cellulose, the effect of lignin residues in the cellulose was examined for the properties and cytocompatibility of the resultant hydrogel films. The cellulose was dissolved in lithium chloride/N,N-dimethylacetamide solution and converted to hydrogel films by phase inversion. In the purification process, sodium hydroxide (NaOH) treatment time was changed from 1 to 12 h. This resulted in cellulose hydrogel films having small amounts of lignin from 1.62 to 0.68%. The remaining lignin greatly affected hydrogel properties. Water content of the hydrogel films was increased from 1153 to 1525% with a decrease of lignin content. Moreover, lower lignin content caused weakening of tensile strength from 0.80 to 0.43 N/mm{sup 2} and elongation from 45.2 to 26.5%. Also, similar tendency was observed in viscoelastic behavior of the cellulose hydrogel films. Evidence was shown that the lignin residue was effective for the high strength of the hydrogel films. In addition, scanning probe microscopy in the morphological observation was suggested that the trace lignin in the cellulose hydrogel affected the cellulose fiber aggregation in the hydrogel network. The trace of lignin in the hydrogels also influenced fibroblast cell culture on the hydrogel films. The hydrogel film containing 1.68% lignin showed better fibroblast compatibility as compared to cell culture polystyrene dish used as reference. - Highlights: • Cellulose hydrogel films with trace lignin were obtained from sugarcane bagasse. • Lignin content was found to be in the range of 1.62 − 0.68% by UV–Vis spectroscopy. • Higher lignin content strengthened mechanical properties of the hydrogel films. • Trace lignin affected the hydrogel morphology such as roughness and porosity. • High cell proliferation was observed in the hydrogel containing 1.68% lignin.

Radiation crosslinking of starch/water-soluble polymer blends for hydrogel

International Nuclear Information System (INIS)

Hashim, K.; Mohid, N.; Bahari, K.; Dahlan, K.Z.

2000-01-01

Water-soluble polymers such as PVP(polyvinyl pyrrolidone) and PVA(polyvinyl alcohol), in aqueous solution can form hydrogel easily upon gamma or electron beam irradiation. The properties of hydrogels, particularly for wound dressing application, can be further improved by adding sago starch to the blend. Results show improved gel strength and elongation properties of the hydrogel with increasing sago concentration. It was found that the PVA/sago hydrogel gives better gel strength and elongation than the PVP/sago hydrogel. The tackiness property of the PVA/sago hydrogel increased with increase amount of sago starch added. In case of PVP/sago hydrogel, the tackiness property shows significant increase with increasing amount of sago except for the 5%PVP composition. The swelling properties of PVP/sago and PVA/sago hydrogel decreased with increasing amount of sago but the crosslink density of the hydrogels also reduced. (author)

Radiation crosslinking of starch/water-soluble polymer blends for hydrogel

Energy Technology Data Exchange (ETDEWEB)

Hashim, K.; Mohid, N.; Bahari, K.; Dahlan, K.Z. [Radiation Processing Technology Division, Malaysian Institute Nuclear Technology Research Malaysia (MINT), Bangi, 43000 Kajang (Malaysia)

2000-03-01

Water-soluble polymers such as PVP(polyvinyl pyrrolidone) and PVA(polyvinyl alcohol), in aqueous solution can form hydrogel easily upon gamma or electron beam irradiation. The properties of hydrogels, particularly for wound dressing application, can be further improved by adding sago starch to the blend. Results show improved gel strength and elongation properties of the hydrogel with increasing sago concentration. It was found that the PVA/sago hydrogel gives better gel strength and elongation than the PVP/sago hydrogel. The tackiness property of the PVA/sago hydrogel increased with increase amount of sago starch added. In case of PVP/sago hydrogel, the tackiness property shows significant increase with increasing amount of sago except for the 5%PVP composition. The swelling properties of PVP/sago and PVA/sago hydrogel decreased with increasing amount of sago but the crosslink density of the hydrogels also reduced. (author)

Trends in World Silk Cocoons and Silk Production and Trade, 2007-2010

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AGATHA AGATHA POPESCU

2013-10-01

Full Text Available The paper aimed to analyze world production and trade for fresh silk cocoons and raw silk using FAO Stat data for  the  period 2007-2010. The use of index, share and comparison methods allowed to identify the major trends in the analyzed period. Silk decline was determined by the increased importance of cotton and artificial fibres in textile and clothing industry. Important changes are taking place on silk cocoons and silk market. While, the European market decreased, the Asian market has mainly developed fresh cocoons and raw silk, while the European market became more interested of clothes. Silk consumption declined because of consumer’s preference for synthetic fibres, except traditional consumers from Asia.  China is the main producer and exporter of fresh and dry cocoons, while raw silk is produced and exported by China, Brazil and Italy and imported by India, Japan and Italy. In Europe, Bulgaria is the top producer of fresh cocoons and raw silk and Italy is the main raw silk importer and the top producer and exporter of textile and fashion clothes. Silk will remain an important raw material for producing high quality and luxury clothes.

Analysis of pH Sensitive Hydrogel Coating Effect to Fiber Bragg Grating Properties for pH Sensor Application

Science.gov (United States)

Yulianti, Ian; Supa'at, Abu Sahmah M.; Idrus, Sevia M.; Kurdi, Ojo

2011-12-01

This paper demonstrates the analysis of fiber Bragg grating properties due to hydrogel coating swelling effect. The modeling was done by simulating the hydrogel swelling behavior, and then carried out strain and stress analysis induced on the fiber due to hydrogel expansion. Meshless numerical method was adopted to solve the Poison Nernst Planck equation coupled to mechanical equation to simulate the hydrogel swelling. The hydrogel coating thickness was varied for 4 values, namely 30 μm, 40 μm, 50 μm and 60 μm. The strain and stress analysis were done numerically using finite element method. The results show that the strain on the fiber increases as the hydrogel coating thickness increased. The increase of hydrogel thickness results in the improvement of sensor sensitivity at the expense of stress value.

Conductive Au nanowires regulated by silk fibroin nanofibers

Science.gov (United States)

Dong, Bo-Ju; Lu, Qiang

2014-03-01

Conductive Au-biopolymer composites have promising applications in tissue engineering such as nerve tissue regeneration. In this study, silk fibroin nanofibers were formed in aqueous solution by regulating silk self-assembly process and then used as template for Au nanowire fabrication. We performed the synthesis of Au seeds by repeating the seeding cycles for several times in order to increase the density of Au seeds on the nanofibers. After electroless plating, densely decorated Au seeds grew into irregularly shaped particles following silk nanofiber to fill the gaps between particles and finally form uniform continuous nanowires. The conductive property of the Au-silk fibroin nanowires was studied with current-voltage ( I-V) measurement. A typical ohmic behavior was observed, which highlighted their potential applications in nerve tissue regeneration.

Investigation of synthetic spider silk crystallinity and alignment via electrothermal, pyroelectric, literature XRD, and tensile techniques.

Science.gov (United States)

Munro, Troy; Putzeys, Tristan; Copeland, Cameron G; Xing, Changhu; Lewis, Randolph V; Ban, Heng; Glorieux, Christ; Wubbenhorst, Michael

2017-04-01

The processes used to create synthetic spider silk greatly affect the properties of the produced fibers. This paper investigates the effect of process variations during artificial spinning on the thermal and mechanical properties of the produced silk. Property values are also compared to the ones of the natural dragline silk of the N. clavipes spider, and to unprocessed (as-spun) synthetic silk. Structural characterization by scanning pyroelectric microscopy is employed to provide insight into the axial orientation of the crystalline regions of the fiber and is supported by XRD data. The results show that stretching and passage through liquid baths induce crystal formation and axial alignment in synthetic fibers, but with different structural organization than natural silks. Furthermore, an increase in thermal diffusivity and elastic modulus is observed with decreasing fiber diameter, trending towards properties of natural fiber. This effect seems to be related to silk fibers being subjected to a radial gradient during production.

The failure mode of natural silk epoxy triggered composite tubes

International Nuclear Information System (INIS)

Eshkour, R A; Ariffin, A K; Zulkifli, R; Sulong, A B; Azhari, C H

2012-01-01

In this study the quasi static compression test over natural silk epoxy triggered composite tubes has been carried out, the natural silk epoxy composite tubes consist of 24 layer of woven natural silk as reinforcement and thermoset epoxy resin as matrix which both of them i e natural silk and epoxy have excellent mechanical properties More over the natural silk have better moisture resistance in comparison with other natural reinforcements, the length of tubes are 50, 80 and 120 mm The natural silk epoxy composite tubes are associated with an external trigger which includes 4 steel pieces welded on downside flat plate fixture The hand lay up fabrication method has been used to make the natural silk epoxy composite tubes Instron universal testing machine with 250 KN load capacity has been employed to accomplish this investigation The failure modes of natural silk epoxy triggered composite tubes has been investigated by representative photographs which has been taken by a high resolution camera(12 2 Mp) during the quasi static compression test, from the photographs is observed the failure modes is progressive local buckling

Preparation of reinforced poly(ethylene oxide) blend hydrogel films containing a drug and assessment of their properties

International Nuclear Information System (INIS)

Yang Zhanshan; Zhu Nankang; Yang Shuqin

1999-01-01

Reinforced poly(ethylene oxide) blend hydrogen films containing mafenide acetate were prepared by using two freezing-thawing cycles and the irradiation crosslinking technique, and their properties and the drug release were assessed. The results showed that the tensile strength of the reinforced PEO blend hydrogel films increased significantly (p < 0.01), the gel fraction and the elongation at break of the films increased slightly as compared with those formed by the irradiation without the freezing-thawing treatment, indicating that the mechanical properties of the PEO blend hydrogel films can be improved by the freezing-thawing cycles. The reinforced films possessed an ideal flexibility, crosslinking density and elasticity as wound dressings. Swelling studies showed that the equilibrium water content of the hydrogel films expressed in the degree of swelling decreased significantly (p < 0.01), suggesting that a significant structural rearrangement of the films occurred during the freezing process. The structural densification resulted in the increase of the mechanical strength of the hydrogel films. The hydrogels formed by the irradiation at doses of 40 kGy were comparatively stronger. Release studies were run on the reinforced hydrogels with mafenide acetate which was incorporated before the freezing-thawing treatment. Release was followed over seven days. The drug transport was controlled by a regular diffusion model

Anisotropic silk fibroin/gelatin scaffolds from unidirectional freezing

Energy Technology Data Exchange (ETDEWEB)

Asuncion, Maria Christine Tankeh, E-mail: christine.asuncion@u.nus.edu [National University of Singapore, Department of Biomedical Engineering (Singapore); Goh, James Cho-Hong [National University of Singapore, Department of Biomedical Engineering (Singapore); National University of Singapore, Department of Orthopedic Surgery (Singapore); Toh, Siew-Lok [National University of Singapore, Department of Biomedical Engineering (Singapore); National University of Singapore, Department of Mechanical Engineering (Singapore)

2016-10-01

Recent studies have underlined the importance of matching scaffold properties to the biological milieu. Tissue, and thus scaffold, anisotropy is one such property that is important yet sometimes overlooked. Methods that have been used to achieve anisotropic scaffolds present challenges such as complicated fabrication steps, harsh processing conditions and toxic chemicals involved. In this study, unidirectional freezing was employed to fabricate anisotropic silk fibroin/gelatin scaffolds in a simple and mild manner. Morphological, mechanical, chemical and cellular compatibility properties were investigated, as well as the effect of the addition of gelatin to certain properties of the scaffold. It was shown that scaffold properties were suitable for cell proliferation and that mesenchymal stem cells were able to align themselves along the directed fibers. The fabricated scaffolds present a platform that can be used for anisotropic tissue engineering applications such as cardiac patches. - Highlights: • Silk/gelatin scaffolds with unidirectional alignment were fabricated using a simple and scalable process • Presence of gelatin in silk resulted to lesser shrinkage, better water retention and improved cell proliferation. • Mesenchymal stem cells were shown to align themselves according to the fiber alignment.

Collagen hydrogels incorporated with surface-aminated mesoporous nanobioactive glass: Improvement of physicochemical stability and mechanical properties is effective for hard tissue engineering.

Science.gov (United States)

El-Fiqi, Ahmed; Lee, Jae Ho; Lee, Eun-Jung; Kim, Hae-Won

2013-12-01

Collagen (Col) hydrogels have poor physicochemical and mechanical properties and are susceptible to substantial shrinkage during cell culture, which limits their potential applications in hard tissue engineering. Here, we developed novel nanocomposite hydrogels made of collagen and mesoporous bioactive glass nanoparticles (mBGns) with surface amination, and addressed the effects of mBGn addition (Col:mBG = 2:1, 1:1 and 1:2) and its surface amination on the physicochemical and mechanical properties of the hydrogels. The amination of mBGn was shown to enable chemical bonding with collagen molecules. As a result, the nanocomposite hydrogels exhibited a significantly improved physicochemical and mechanical stability. The hydrolytic and enzymatic degradation of the Col-mBGn hydrogels were slowed down due to the incorporation of mBGn and its surface amination. The mechanical properties of the hydrogels, specifically the resistance to loading as well as the stiffness, significantly increased with the addition of mBGn and its aminated form, as assessed by a dynamic mechanical analysis. Mesenchymal stem cells cultivated within the Col-mBGn hydrogels were highly viable, with enhanced cytoskeletal extensions, due to the addition of surface aminated mBGn. While the Col hydrogel showed extensive shrinkage (down to ∼20% of initial size) during a few days of culture, the shrinkage of the mBGn-added hydrogel was substantially reduced, and the aminated mBGn-added hydrogel had no observable shrinkage over 21 days. Results demonstrated the effective roles of aminated mBGn in significantly improving the physicochemical and mechanical properties of Col hydrogel, which are ultimately favorable for applications in stem cell culture for bone tissue engineering. Copyright © 2013 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Control of the rheological properties of clay nanosheet hydrogels with a guanidinium-attached calix[4]arene binder.

Science.gov (United States)

Lee, Ji Ha; Kim, Chaelin; Jung, Jong Hwa

2015-10-21

A 1,3-alternate calix[4]arene derivative 1 possessing four guanidinium moieties was synthesized as a molecular binder. The clay nanosheet (CNS) hydrogels were prepared upon addition of 1 and sodium polyacrylate (ASSP), and their mechanical properties were measured by rheometry. CNS hydrogels prepared by combining calix[4]arene 1 with dispersed CNSs surrounded by ASSPs showed an enhancement of mechanical properties such as viscosity and elasticity.

The effect of hirudin modification of silk fibroin on cell growth and antithrombogenicity

Energy Technology Data Exchange (ETDEWEB)

Wang, Qiongyu; Tu, Fangfang; Liu, Yunfei; Zhang, Yujin; Li, Helei; Kang, Zhao [National Engineering Laboratory for Modern Silk, College of Textile and Clothing Engineering, Soochow University, No. 199 Ren-ai Road, Suzhou Industrial Park, Suzhou, Jiangsu Province 215123 (China); Yin, Yin [Laboratory Animal Research Center, Soochow University, Suzhou, Jiangsu 215123 (China); Wang, Jiannan, E-mail: wangjn@suda.edu.cn [National Engineering Laboratory for Modern Silk, College of Textile and Clothing Engineering, Soochow University, No. 199 Ren-ai Road, Suzhou Industrial Park, Suzhou, Jiangsu Province 215123 (China)

2017-06-01

Thrombus formation remains a particular challenge for small-diameter vascular grafts. In this study, the direct thrombin inhibitor hirudin (Hir) was used to modify silk fibroin films in an attempt to enhance its antithrombogenic properties. Hir was successfully attached to silk fibroin and uniformly distributed in the regenerative material. Hir-modified films showed good cytocompatibility, and supported adhesion and proliferation of fibroblasts (L929), human umbilical vascular endothelial cells (HUVECs) and human aortic smooth muscle cells (HASMCs). Proliferation of HAVSMCs was inhibited by increasing Hir concentration. Activated partial thrombin time (APTT), prothrombin time (PT) and thrombin time (TT) of Hir-modified silk fibroin tubular scaffolds (SFTSs) were all increased markedly compared with fresh rabbit blood, ethanol-treated SFTS and unmodified SFTS, demonstrating the improved antithrombogenicity of SFTSs following modification with Hir. - Highlights: • A direct thrombin inhibitor hirudin was used to modify silk fibroin. • Antithrombogenic property of Hir-modified silk fibroin films was improved. • Hir-modified silk fibroin films supported adhesion and proliferation of HUVECs and HAVSMCs. • Proliferation of HAVSMCs on silk fibroin films was inhibited by increasing Hir concentration.

Radiation degradation of silk

Energy Technology Data Exchange (ETDEWEB)

Ishida, Kazushige; Kamiishi, Youichi [Textile Research Institute of Gunma, Kiryu, Gunma (Japan); Takeshita, Hidefumi; Yoshii, Fumio; Kume, Tamikazu [Japan Atomic Energy Research Inst., Takasaki, Gunma (Japan). Takasaki Radiation Chemistry Research Establishment

2001-03-01

Silk fibroin powder was prepared from irradiated silk fibroin fiber by means of only physical treatment. Silk fibroin fiber irradiated with an accelerated electron beam in the dose range of 250 - 1000 kGy was pulverized by using a ball mill. Unirradiated silk fibroin fiber was not pulverized at all. But the more irradiation was increased, the more the conversion efficiency from fiber to powder was increased. The conversion efficiency of silk fibroin fiber irradiated 1000 kGy in oxygen was 94%. Silk fibroin powder shows remarkable solubility, which dissolved 57% into water of ambient temperature. It is a very interesting phenomenon that silk fibroin which did not treat with chemicals gets solubility only being pulverized. In order to study mechanism of solubilization of silk fibroin powder, amino acid component of soluble part of silk fibroin powder was analyzed. The more irradiation dose up, the more glycine or alanine degraded, but degradation fraction reached bounds about 50%. Other amino acids were degraded only 20% even at the maximum. To consider crystal construction of silk fibroin, it is suggested that irradiation on silk fibroin fiber selectively degrades glycine and alanine in amorphous region, which makes it possible to pulverize and to dissolve silk fibroin powder. (author)

Preparation and Properties of 3D Printed Alginate–Chitosan Polyion Complex Hydrogels for Tissue Engineering

Directory of Open Access Journals (Sweden)

Qiongqiong Liu

2018-06-01

Full Text Available Three-dimensional (3D printing holds great potential for preparing sophisticated scaffolds for tissue engineering. As a result of the shear thinning properties of an alginate solution, it is often used as 3D printing ink. However, it is difficult to prepare scaffolds with complexity structure and high fidelity, because the alginate solution has a low viscosity and alginate hydrogels prepared with Ca2+ crosslinking are mechanically weak. In this work, chitosan powders were dispersed and swelled in an alginate solution, which could effectively improve the viscosity of an alginate solution by 1.5–4 times. With the increase of chitosan content, the shape fidelity of the 3D printed alginate–chitosan polyion complex (AlCh PIC hydrogels were improved. Scanning electron microscope (SEM photographs showed that the lateral pore structure of 3D printed hydrogels was becoming more obvious. As a result of the increased reaction ion pairs in comparison to the alginate hydrogels that were prepared with Ca2+ crosslinking, AlCh PIC hydrogels were mechanically strong, and the compression stress of hydrogels at a 90% strain could achieve 1.4 MPa without breaking. In addition, human adipose derived stem cells (hASCs adhered to the 3D printed AlCh PIC hydrogels and proliferated with time, which indicated that the obtained hydrogels were biocompatible and could potentially be used as scaffolds for tissue engineering.

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

Science.gov (United States)

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.

Regeneration of Bombyx mori silk nanofibers and nanocomposite fibrils by the electrospinning process

Science.gov (United States)

Ayutsede, Jonathan Eyitouyo

In recent years, there has been significant interest in the utilization of natural materials for novel nanoproducts such as tissue engineered scaffolds. Silkworm silk fibers represent one of the strongest natural fibers known. Silkworm silk, a protein-based natural biopolymer, has received renewed interest in recent years due to its unique properties (strength, toughness) and potential applications such as smart textiles, protective clothing and tissue engineering. The traditional 10--20 mum diameter, triangular-shaped Bombyx mori fibers have remained unchanged over the years. However, in our study, we examine the scientific implication and potential applications of reducing the diameter to the nanoscale, changing the triangular shape of the fiber and adding nanofillers in the form of single wall carbon nanotubes (SWNT) by the electrospinning process. The electrospinning process preserves the natural conformation of the silk (random and beta-sheet). The feasibility of changing the properties of the electrospun nanofibers by post processing treatments (annealing and chemical treatment) was investigated. B. mori silk fibroin solution (formic acid) was successfully electrospun to produce uniform nanofibers (as small as 12 nm). Response Surface Methodology (RSM) was applied for the first time to experimental results of electrospinning, to develop a processing window that can reproduce regenerated silk nanofibers of a predictable size (d silk multifunctional nanocomposite fibers were fabricated for the first time with anticipated properties (mechanical, thermal and electrically conductive) that may have scientific applications (nerve regeneration, stimulation of cell-scaffold interaction). In order to realize these applications, the following areas need to be addressed: a systematic investigation of the dispersion of the nanotubes in the silk matrix, a determination of new methodologies for characterizing the nanofiber properties and establishing the nature of the silk

Electrodeposited silk coatings for functionalized implant applications

Science.gov (United States)

Elia, Roberto

The mechanical and morphological properties of titanium as well as its biocompatibility and osteoinductive characteristics have made it the material of choice for dental implant systems. Although the success rate of titanium implants exceeds 90% in healthy individuals, a large subset of the population has one or more risk factors that inhibit implant integration. Treatments and coatings have been developed to improve clinical outcomes via introduction of appropriate surface topography, texture and roughness or incorporation of bioactive molecules. It is essential that the coatings and associated deposition techniques are controllable and reproducible. Currently, methods of depositing functional coatings are dictated by numerous parameters (temperature, particle size distribution, pH and voltage), which result in variable coating thickness, strength, porosity and weight, and hinder or preclude biomolecule incorporation. Silk is a highly versatile protein with a unique combination of mechanical and physical properties, including tunable degradation, biocompatibility, drug stabilizing capabilities and mechanical properties. Most recently an electrogelation technique was developed which allows for the deposition of gels which dry seamlessly over the contoured topography of the conductive substrate. In this work we examine the potential use of silk electrogels as mechanically robust implant coatings capable of sequestering and releasing therapeutic agents. Electrodeposition of silk electrogels formed in uniform electric fields was characterized with respect to field intensity and deposition time. Gel formation kinetics were used to derive functions which allowed for the prediction of coating deposition over a range of process and solution parameters. Silk electrogel growth orientation was shown to be influenced by the applied electric field. Coatings were reproducible and tunable via intrinsic silk solution properties and extrinsic process parameters. Adhesion was

Role of chondroitin sulphate tethered silk scaffold in cartilaginous disc tissue regeneration.

Science.gov (United States)

Bhattacharjee, Maumita; Chawla, Shikha; Chameettachal, Shibu; Murab, Sumit; Bhavesh, Neel Sarovar; Ghosh, Sourabh

2016-04-12

Strategies for tissue engineering focus on scaffolds with tunable structure and morphology as well as optimum surface chemistry to simulate the anatomy and functionality of the target tissue. Silk fibroin has demonstrated its potential in supporting cartilaginous tissue formation both in vitro and in vivo. In this study, we investigate the role of controlled lamellar organization and chemical composition of biofunctionalized silk scaffolds in replicating the structural properties of the annulus region of an intervertebral disc using articular chondrocytes. Covalent attachment of chondroitin sulfate (CS) to silk is characterized. CS-conjugated silk constructs demonstrate enhanced cellular metabolic activity and chondrogenic redifferentiation potential with significantly improved mechanical properties over silk-only constructs. A matrix-assisted laser desorption ionization-time of flight analysis and protein-protein interaction studies help to generate insights into how CS conjugation can facilitate the production of disc associated matrix proteins, compared to a silk-only based construct. An in-depth understanding of the interplay between such extra cellular matrix associated proteins should help in designing more rational scaffolds for cartilaginous disc regeneration needs.

Role of chondroitin sulphate tethered silk scaffold in cartilaginous disc tissue regeneration

International Nuclear Information System (INIS)

Bhattacharjee, Maumita; Chawla, Shikha; Chameettachal, Shibu; Murab, Sumit; Ghosh, Sourabh; Bhavesh, Neel Sarovar

2016-01-01

Strategies for tissue engineering focus on scaffolds with tunable structure and morphology as well as optimum surface chemistry to simulate the anatomy and functionality of the target tissue. Silk fibroin has demonstrated its potential in supporting cartilaginous tissue formation both in vitro and in vivo. In this study, we investigate the role of controlled lamellar organization and chemical composition of biofunctionalized silk scaffolds in replicating the structural properties of the annulus region of an intervertebral disc using articular chondrocytes. Covalent attachment of chondroitin sulfate (CS) to silk is characterized. CS-conjugated silk constructs demonstrate enhanced cellular metabolic activity and chondrogenic redifferentiation potential with significantly improved mechanical properties over silk-only constructs. A matrix-assisted laser desorption ionization-time of flight analysis and protein–protein interaction studies help to generate insights into how CS conjugation can facilitate the production of disc associated matrix proteins, compared to a silk-only based construct. An in-depth understanding of the interplay between such extra cellular matrix associated proteins should help in designing more rational scaffolds for cartilaginous disc regeneration needs. (paper)

Tunable green graphene-silk biomaterials: Mechanism of protein-based nanocomposites.

Science.gov (United States)

Wang, Fang; Jyothirmayee Aravind, S S; Wu, Hao; Forys, Joseph; Venkataraman, Venkat; Ramanujachary, Kandalam; Hu, Xiao

2017-10-01

Green graphene materials prepared by photoreduction of graphite oxide were first time blended with aqueous-based silk fibroin proteins to improve the mechanical and thermal properties of silk biomaterials, and their nanocomposite interaction mechanism was illustrated. Powder X-ray diffraction (XRD) analysis confirmed the complete exfoliation of graphite oxide to graphene in presence of focused pulses of solar radiation. By varying the concentration of graphene (0.1wt% to 10wt%), a series of free standing graphene-silk films were prepared and were systematically characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and nanoindentation measurements. The homogeneity of graphene in silk as well as the thermal stability of the composite films was demonstrated by thermal gravimetric analysis (TGA) and temperature-modulated differential scanning calorimetry (TMDSC). Surprisingly, silk composite film containing only 0.5wt% of graphene gives the highest Young's modulus of 1.65GPa (about 5.8 times higher than the pure silk's modulus), indicating a nano-composite to micro-composite transition of silk-graphene structure occurred around this mixing ratio. This finding provided an easy approach to improve the elastic modulus and other physical properties of silk materials by adding a tiny amount of graphene sheets. Fibroblast cells studies also proved that these graphene-silk materials can significantly improve cell adhesion, growth and proliferation. This protein nanocomposite study provided a useful model to understand how to manipulate the hydrophobic-hydrophobic and polar-polar interactions between high-surface-area inorganic nanomaterials and amphiphilic protein materials, which has many emerging applications in the material science and engineering, such as bio-device fabrication, drug storage and release, and tissue regeneration. Copyright © 2017 Elsevier B.V. All rights reserved.

Characterization and assembly of a GFP-tagged cylindriform silk into hexameric complexes.

Science.gov (United States)

Öster, Carl; Svensson Bonde, Johan; Bülow, Leif; Dicko, Cedric

2014-04-01

Spider silk has been studied extensively for its attractive mechanical properties and potential applications in medicine and industry. The production of spider silk, however, has been lagging behind for lack of suitable systems. Our approach focuses on solving the production of spider silk by designing, expressing, purifying and characterizing the silk from cylindriform glands. We show that the cylindriform silk protein, in contrast to the commonly used dragline silk protein, is fully folded and stable in solution. With the help of GFP as a fusion tag we enhanced the expression of the silk protein in Escherichia coli and could optimize the downstream processing. Secondary structures analysis by circular dichroism and FTIR shows that the GFP-silk fusion protein is predominantly α-helical, and that pH can trigger a α- to β-transition resulting in aggregation. Structural analysis by small angle X-ray scattering suggests that the GFP-Silk exists in the form of a hexamer in solution. Copyright © 2013 Wiley Periodicals, Inc.

Device for simultaneous measurements of the optical and dielectric properties of hydrogels

International Nuclear Information System (INIS)

Gómez-Galván, F; Lara-Ceniceros, T; Mercado-Uribe, H

2012-01-01

We have designed an experimental device to simultaneously measure the light transmittance and dielectric properties of thermo-sensitive hydrogels. We have used this device to study poly(N-isopropylacrylamide) samples in order to understand the mechanism of water deliverance during the phase transition such hydrogels normally exhibit. We found that the phase transition can be observed dielectrically at low frequencies, when the isothermals obtained during the heating of the samples separate into two groups. The phenomenon occurs due to the increase of ions caused by the dissociation of water molecules released by the polymer, and corresponds to the drop of the optical transmittance

Spider Silk Processing for Spidroin Recovery from Crossopriza Lyoni Web

Science.gov (United States)

Mohtar, J. A.; Ooi, W. L.; Yusuf, F.

2018-03-01

Spider silk is a potential biomaterial that can be used in various applications for its outstanding physicomechanical properties attributed by the spidroin composition. Efforts for commercializing spider silks have been mainly focused on the characterization of spidroins from the Entelegyne spiders for exceptional fibre construction. Hence, studies on silk proteins from the Haplogyne species remain neglected. The aim of this study is to isolate spidroin from Crossopriza lyoni web. Silk processing involved the pretreatment of fibres for the shell layer removal from the surface. A screening study was conducted to analyze the effect of temperature, incubation time and agitation speed on spidroin extraction using Ajisawa’s reagent by OFAT analysis followed by statistical optimization of the extraction process via RSM for maximal protein recovery. All parameters exerted significant effect on spidroin recovery (pspider silk to meet the demand for a variety of silk-based products in the near future.

[Engineered spider silk: the intelligent biomaterial of the future. Part I].

Science.gov (United States)

Florczak, Anna; Piekoś, Konrad; Kaźmierska, Katarzyna; Mackiewicz, Andrzej; Dams-Kozłowska, Hanna

2011-06-17

The unique properties of spider silk such as strength, extensibility, toughness, biocompatibility and biodegradability are the reasons for the recent development in silk biomaterial technology. For a long time scientific progress was impeded by limited access to spider silk. However, the development of the molecular biology strategy was a breaking point in synthetic spider silk protein design. The sequences of engineered spider silk are based on the consensus motives of the corresponding natural equivalents. Moreover, the engineered silk proteins may be modified in order to gain a new function. The strategy of the hybrid proteins constructed on the DNA level combines the sequence of engineered silk, which is responsible for the biomaterial structure, with the sequence of polypeptide which allows functionalization of the silk biomaterial. The functional domains may comprise receptor binding sites, enzymes, metal or sugar binding sites and others. Currently, advanced research is being conducted, which on the one hand focuses on establishing the particular silk structure and understanding the process of silk thread formation in nature. On the other hand, there are attempts to improve methods of engineered spider silk protein production. Due to acquired knowledge and recent progress in synthetic protein technology, the engineered silk will turn into intelligent biomaterial of the future, while its industrial production scale will trigger a biotechnological revolution.

Silk elasticity as a potential constraint on spider body size.

Science.gov (United States)

Rodríguez-Gironés, Miguel A; Corcobado, Guadalupe; Moya-Laraño, Jordi

2010-10-07

Silk is known for its strength and extensibility and has played a key role in the radiation of spiders. Individual spiders use different glands to produce silk types with unique sets of proteins. Most research has studied the properties of major ampullate and capture spiral silks and their ecological implications, while little is known about minor ampullate silk, the type used by those spider species studied to date for bridging displacements. A biomechanical model parameterised with available data shows that the minimum radius of silk filaments required for efficient bridging grows with the square root of the spider's body mass, faster than the radius of minor ampullate silk filaments actually produced by spiders. Because the morphology of spiders adapted to walking along or under silk threads is ill suited for moving on a solid surface, for these species there is a negative relationship between body mass and displacement ability. As it stands, the model suggests that spiders that use silk for their displacements are prevented from attaining a large body size if they must track their resources in space. In particular, silk elasticity would favour sexual size dimorphism because males that must use bridging lines to search for females cannot grow large. 2010 Elsevier Ltd. All rights reserved.

Ionic Conductivity of Polyelectrolyte Hydrogels.

Science.gov (United States)

Lee, Chen-Jung; Wu, Haiyan; Hu, Yang; Young, Megan; Wang, Huifeng; Lynch, Dylan; Xu, Fujian; Cong, Hongbo; Cheng, Gang

2018-02-14

Polyelectrolytes have many important functions in both living organisms and man-made applications. One key property of polyelectrolytes is the ionic conductivity due to their porous networks that allow the transport of water and small molecular solutes. Among polyelectrolytes, zwitterionic polymers have attracted huge attention for applications that involve ion transport in a polyelectrolyte matrix; however, it is still unclear how the functional groups of zwitterionic polymer side chains affect their ion transport and swelling properties. In this study, zwitterionic poly(carboxybetaine acrylamide), poly(2-methacryloyloxyethyl phosphorylcholine), and poly(sulfobetaine methacrylate) hydrogels were synthesized and their ionic conductivity was studied and compared to cationic, anionic, and nonionic hydrogels. The change of the ionic conductivity of zwitterionic and nonionic hydrogels in different saline solutions was investigated in detail. Zwitterionic hydrogels showed much higher ionic conductivity than that of the widely used nonionic poly(ethylene glycol) methyl ether methacrylate hydrogel in all tested solutions. For both cationic and anionic hydrogels, the presence of mobile counterions led to high ionic conductivity in low salt solutions; however, the ionic conductivity of zwitterionic hydrogels surpassed that of cationic and ionic hydrogels in high salt solutions. Cationic and anionic hydrogels showed much higher water content than that of zwitterionic hydrogels in deionized water; however, the cationic hydrogels shrank significantly with increasing saline concentration. This work provides insight into the effects of polyelectrolyte side chains on ion transport. This can guide us in choosing better polyelectrolytes for a broad spectrum of applications, including bioelectronics, neural implants, battery, and so on.

Silk scaffolds in bone tissue engineering: An overview.

Science.gov (United States)

Bhattacharjee, Promita; Kundu, Banani; Naskar, Deboki; Kim, Hae-Won; Maiti, Tapas K; Bhattacharya, Debasis; Kundu, Subhas C

2017-11-01

Bone tissue plays multiple roles in our day-to-day functionality. The frequency of accidental bone damage and disorder is increasing worldwide. Moreover, as the world population continues to grow, the percentage of the elderly population continues to grow, which results in an increased number of bone degenerative diseases. This increased elderly population pushes the need for artificial bone implants that specifically employ biocompatible materials. A vast body of literature is available on the use of silk in bone tissue engineering. The current work presents an overview of this literature from materials and fabrication perspective. As silk is an easy-to-process biopolymer; this allows silk-based biomaterials to be molded into diverse forms and architectures, which further affects the degradability. This makes silk-based scaffolds suitable for treating a variety of bone reconstruction and regeneration objectives. Silk surfaces offer active sites that aid the mineralization and/or bonding of bioactive molecules that facilitate bone regeneration. Silk has also been blended with a variety of polymers and minerals to enhance its advantageous properties or introduce new ones. Several successful works, both in vitro and in vivo, have been reported using silk-based scaffolds to regenerate bone tissues or other parts of the skeletal system such as cartilage and ligament. A growing trend is observed toward the use of mineralized and nanofibrous scaffolds along with the development of technology that allows to control scaffold architecture, its biodegradability and the sustained releasing property of scaffolds. Further development of silk-based scaffolds for bone tissue engineering, taking them up to and beyond the stage of human trials, is hoped to be achieved in the near future through a cross-disciplinary coalition of tissue engineers, material scientists and manufacturing engineers. The state-of-art of silk biomaterials in bone tissue engineering, covering their wide

Cytocompatibility of a silk fibroin tubular scaffold

International Nuclear Information System (INIS)

Wang, Jiannan; Wei, Yali; Yi, Honggen; Liu, Zhiwu; Sun, Dan; Zhao, Huanrong

2014-01-01

Regenerated silk fibroin (SF) materials are increasingly used for tissue engineering applications. In order to explore the feasibility of a novel biomimetic silk fibroin tubular scaffold (SFTS) crosslinked by poly(ethylene glycol) diglycidyl ether (PEG-DE), biocompatibility with cells was evaluated. The novel biomimetic design of the SFTS consisted of three distinct layers: a regenerated SF intima, a silk braided media and a regenerated SF adventitia. The SFTS exhibited even silk fibroin penetration throughout the braid, forming a porous layered tube with superior mechanical, permeable and cell adhesion properties that are beneficial to vascular regeneration. Cytotoxicity and cell compatibility were tested on L929 cells and human umbilical vein endothelial cells (EA.hy926). DNA content analysis, scanning electron and confocal microscopies and MTT assay showed no inhibitory effects on DNA replication. Cell morphology, viability and proliferation were good for L929 cells, and satisfactory for EA.hy926 cells. Furthermore, the suture retention strength of the SFTS was about 23 N and the Young's modulus was 0.2–0.3 MPa. Collectively, these data demonstrate that PEG-DE crosslinked SFTS possesses the appropriate cytocompatibility and mechanical properties for use as vascular scaffolds as an alternative to vascular autografts. - Highlights: • A PEG-DE cross-linked small caliber porous silk fibroin tubular scaffold (SFTS) • PEG-DE cross-linked SF film had no inhibitory effect on DNA replication of cells. • Cells cultured on the SFTS showed good morphology, cell viability and proliferative activity. • SFTS would be beneficial to endothelialization. • SFTS had good suture retention strength and flexibility

Genetic engineered color silk: fabrication of a photonics material through a bioassisted technology.

Science.gov (United States)

Shimizu, Katsuhiko

2018-05-15

Silk produced by the silkworm Bombyx mori is an attractive material because of its luster, smooth and soft texture, conspicuous mechanical strength, good biocompatibility, slow biodegradation, and carbon neutral synthesis. Silkworms have been domesticated and bred for production of better quality and quantity of silk, resulting in the development of sericulture and the textile industry. Silk is generally white, so dyeing is required to obtain colored fiber. However, the dyeing process involves harsh conditions and generates a large volume of waste water, which have environmentally and economically negative impacts. Although some strains produce cocoons that contain pigments derived from the mulberry leaves that they eat, the pigments are distributed in the sericin layer and are lost during gumming. In trials for production of colored silk by feeding silkworms on diets containing dyes, only limited species of dye molecules were incorporated into the silk threads. A method for the generation of transgenic silkworm was established in conjunction with the discovery of green fluorescent protein (GFP), and silkworms carrying the GFP gene spun silk threads that formed cocoons that glowed bright green and still retained the original properties of silk. A wide range of color variation of silk threads has been obtained by replacing the GFP gene with the genes of other fluorescent proteins chosen from the fluorescent protein palette. The genetically modified silk with photonic properties can be processed to form various products including linear threads, 2D fabrics, and 3D materials. The transgenic colored silk could be economically advantageous due to addition of a new value to silk and reduction of cost for water waste, and environmentally preferable for saving water. Here, I review the literature regarding the production methods of fluorescent silk from transgenic silkworms and present examples of genetically modified color silk.

Improved human tenocyte proliferation and differentiation in vitro by optimized silk degumming

Energy Technology Data Exchange (ETDEWEB)

Wang Xiao; Qiu Yiwei; Carr, Andrew J; Triffitt, James T; Sabokbar, Afsie; Xia Zhidao, E-mail: z.xia@swansea.ac.uk [Botnar Research Centre, Nuffield Department of Orthopaedics, Rheumatology and Musculoskeletal Sciences, University of Oxford, Oxford (United Kingdom)

2011-06-15

Tendon disorders are common clinical conditions. Tendon tissue engineering provides a new approach for tendon repair by integrating engineered substitutes with their native counterparts. Silk is considered to be a promising candidate for tendon engineering because of its biological and mechanical properties. However, a major concern with using silk for biomedical applications is the immune responses generated by sericin, a glue-like protein that coats the silk fibres. This study improves the existing protocols for silk 'degumming' which removes sericin and enables preparation of silk that is suitable for tendon regeneration. Bombyx mori silks were treated by sequential treatments with different proteases. The efficiency of degumming was determined by measuring weight loss, picric acid and carmine staining and scanning electron microscopy. To evaluate the cellular responses after degumming, the growth and differentiation of human tenocytes on silks were examined. The results showed that sequential protease treatment effectively degummed raw silks. The sequentially degummed silks showed enhanced tenocyte proliferation and upregulated mRNA levels of tendon markers. Thick cell multilayers formed on the treated silks, with cells and collagen fibres penetrating into the spaces in individual silk filaments, resulting in a structure resembling human tendon.

Improved human tenocyte proliferation and differentiation in vitro by optimized silk degumming

Energy Technology Data Exchange (ETDEWEB)

Xiao, Wang; Yiwei, Qiu; Carr, Andrew J; Triffitt, James T; Sabokbar, Afsie; Xia Zhidao, E-mail: z.xia@swansea.ac.uk [Botnar Research Centre, Nuffield Department of Orthopaedics, Rheumatology and Musculoskeletal Sciences, University of Oxford, Oxford (United Kingdom)

2011-06-15

Tendon disorders are common clinical conditions. Tendon tissue engineering provides a new approach for tendon repair by integrating engineered substitutes with their native counterparts. Silk is considered to be a promising candidate for tendon engineering because of its biological and mechanical properties. However, a major concern with using silk for biomedical applications is the immune responses generated by sericin, a glue-like protein that coats the silk fibres. This study improves the existing protocols for silk 'degumming' which removes sericin and enables preparation of silk that is suitable for tendon regeneration. Bombyx mori silks were treated by sequential treatments with different proteases. The efficiency of degumming was determined by measuring weight loss, picric acid and carmine staining and scanning electron microscopy. To evaluate the cellular responses after degumming, the growth and differentiation of human tenocytes on silks were examined. The results showed that sequential protease treatment effectively degummed raw silks. The sequentially degummed silks showed enhanced tenocyte proliferation and upregulated mRNA levels of tendon markers. Thick cell multilayers formed on the treated silks, with cells and collagen fibres penetrating into the spaces in individual silk filaments, resulting in a structure resembling human tendon.

Optical surface profiling of orb-web spider capture silks

Energy Technology Data Exchange (ETDEWEB)

Kane, D M; Joyce, A M; Staib, G R [Department of Physics, Macquarie University, Sydney, NSW 2109 (Australia); Herberstein, M E, E-mail: deb.kane@mq.edu.a [Department of Biological Sciences, Macquarie University, Sydney, NSW 2109 (Australia)

2010-09-15

Much spider silk research to date has focused on its mechanical properties. However, the webs of many orb-web spiders have evolved for over 136 million years to evade visual detection by insect prey. It is therefore a photonic device in addition to being a mechanical device. Herein we use optical surface profiling of capture silks from the webs of adult female St Andrews cross spiders (Argiope keyserlingi) to successfully measure the geometry of adhesive silk droplets and to show a bowing in the aqueous layer on the spider capture silk between adhesive droplets. Optical surface profiling shows geometric features of the capture silk that have not been previously measured and contributes to understanding the links between the physical form and biological function. The research also demonstrates non-standard use of an optical surface profiler to measure the maximum width of a transparent micro-sized droplet (microlens).

Optical surface profiling of orb-web spider capture silks

International Nuclear Information System (INIS)

Kane, D M; Joyce, A M; Staib, G R; Herberstein, M E

2010-01-01

Much spider silk research to date has focused on its mechanical properties. However, the webs of many orb-web spiders have evolved for over 136 million years to evade visual detection by insect prey. It is therefore a photonic device in addition to being a mechanical device. Herein we use optical surface profiling of capture silks from the webs of adult female St Andrews cross spiders (Argiope keyserlingi) to successfully measure the geometry of adhesive silk droplets and to show a bowing in the aqueous layer on the spider capture silk between adhesive droplets. Optical surface profiling shows geometric features of the capture silk that have not been previously measured and contributes to understanding the links between the physical form and biological function. The research also demonstrates non-standard use of an optical surface profiler to measure the maximum width of a transparent micro-sized droplet (microlens).

Synthesis and properties of regenerated cellulose-based hydrogels with high strength and transparency for potential use as an ocular bandage

International Nuclear Information System (INIS)

Patchan, M.; Graham, J.L.; Xia, Z.; Maranchi, J.P.; McCally, R.; Schein, O.; Elisseeff, J.H.; Trexler, M.M.

2013-01-01

Cellulose is a biologically derived material with excellent wound-healing properties. The high strength of cellulose fibers and the ability to synthesize gels with high optical transparency make these materials suitable for ocular applications. In this study, cellulose materials derived from wood pulp, cotton, and bacterial sources were dissolved in lithium chloride/N,N-dimethylacetamide to form regenerated cellulose hydrogels. Material properties of the resulting hydrogels, including water content, optical transparency, and tensile and tear strengths, were evaluated. Synthesis parameters, including activation time, dissolution time, relative humidity, and cellulose concentration, were found to impact the material properties of the resulting hydrogels. Overnight activation time improves the optical transparency of the hydrogels from 77% to 97% at 550 nm, whereas controlling cellulose concentration improves their tear strength by as much as 200%. On the basis of the measured transmittance and strength values of the regenerated hydrogels prepared via the optimized synthesis parameters, Avicel PH 101, Sigma-Aldrich microcrystalline cellulose 435236, and bacterial cellulose types were prioritized for future biocompatibility testing and potential clinical investigation. - Highlights: • Hydrogels were prepared (via LiCl/DMAc) from 7 different types of cellulose. • Synthesis parameters (activation, gelation, and concentration) were optimized. • Impact of synthesis parameters on transparency and strength was explored

Synthesis and properties of regenerated cellulose-based hydrogels with high strength and transparency for potential use as an ocular bandage

Energy Technology Data Exchange (ETDEWEB)

Patchan, M. [Research and Exploratory Development Department, The Johns Hopkins University Applied Physics Laboratory, 11100 Johns Hopkins Road, Laurel, MD 20723 (United States); Graham, J.L. [Department of Biomedical Engineering, Johns Hopkins University, School of Medicine, 720 Rutland Avenue/Ross 720, Baltimore, MD 21205 (United States); Xia, Z.; Maranchi, J.P. [Research and Exploratory Development Department, The Johns Hopkins University Applied Physics Laboratory, 11100 Johns Hopkins Road, Laurel, MD 20723 (United States); McCally, R. [Research and Exploratory Development Department, The Johns Hopkins University Applied Physics Laboratory, 11100 Johns Hopkins Road, Laurel, MD 20723 (United States); Wilmer Eye Institute, Johns Hopkins Medical Institutions, 600 N. Wolfe Street, Baltimore, MD 21287 (United States); Schein, O. [Wilmer Eye Institute, Johns Hopkins Medical Institutions, 600 N. Wolfe Street, Baltimore, MD 21287 (United States); Elisseeff, J.H. [Department of Biomedical Engineering, Johns Hopkins University, School of Medicine, 720 Rutland Avenue/Ross 720, Baltimore, MD 21205 (United States); Trexler, M.M., E-mail: morgana.trexler@jhuapl.edu [Research and Exploratory Development Department, The Johns Hopkins University Applied Physics Laboratory, 11100 Johns Hopkins Road, Laurel, MD 20723 (United States)

2013-07-01

Cellulose is a biologically derived material with excellent wound-healing properties. The high strength of cellulose fibers and the ability to synthesize gels with high optical transparency make these materials suitable for ocular applications. In this study, cellulose materials derived from wood pulp, cotton, and bacterial sources were dissolved in lithium chloride/N,N-dimethylacetamide to form regenerated cellulose hydrogels. Material properties of the resulting hydrogels, including water content, optical transparency, and tensile and tear strengths, were evaluated. Synthesis parameters, including activation time, dissolution time, relative humidity, and cellulose concentration, were found to impact the material properties of the resulting hydrogels. Overnight activation time improves the optical transparency of the hydrogels from 77% to 97% at 550 nm, whereas controlling cellulose concentration improves their tear strength by as much as 200%. On the basis of the measured transmittance and strength values of the regenerated hydrogels prepared via the optimized synthesis parameters, Avicel PH 101, Sigma-Aldrich microcrystalline cellulose 435236, and bacterial cellulose types were prioritized for future biocompatibility testing and potential clinical investigation. - Highlights: • Hydrogels were prepared (via LiCl/DMAc) from 7 different types of cellulose. • Synthesis parameters (activation, gelation, and concentration) were optimized. • Impact of synthesis parameters on transparency and strength was explored.

Precisely printable and biocompatible silk fibroin bioink for digital light processing 3D printing.

Science.gov (United States)

Kim, Soon Hee; Yeon, Yeung Kyu; Lee, Jung Min; Chao, Janet Ren; Lee, Young Jin; Seo, Ye Been; Sultan, Md Tipu; Lee, Ok Joo; Lee, Ji Seung; Yoon, Sung-Il; Hong, In-Sun; Khang, Gilson; Lee, Sang Jin; Yoo, James J; Park, Chan Hum

2018-04-24

Although three-dimensional (3D) bioprinting technology has gained much attention in the field of tissue engineering, there are still several significant engineering challenges to overcome, including lack of bioink with biocompatibility and printability. Here, we show a bioink created from silk fibroin (SF) for digital light processing (DLP) 3D bioprinting in tissue engineering applications. The SF-based bioink (Sil-MA) was produced by a methacrylation process using glycidyl methacrylate (GMA) during the fabrication of SF solution. The mechanical and rheological properties of Sil-MA hydrogel proved to be outstanding in experimental testing and can be modulated by varying the Sil-MA contents. This Sil-MA bioink allowed us to build highly complex organ structures, including the heart, vessel, brain, trachea and ear with excellent structural stability and reliable biocompatibility. Sil-MA bioink is well-suited for use in DLP printing process and could be applied to tissue and organ engineering depending on the specific biological requirements.

Biomaterials Derived from Silk-Tropoelastin Protein Systems

Science.gov (United States)

Hu, Xiao; Wang, Xiuli; Rnjak, Jelena; Weiss, Anthony S.; Kaplan, David L.

2010-01-01

A structural protein blend system based on silkworm silk fibroin and recombinant human tropoelastin is described. Silk fibroin, a semicrystalline fibrous protein with beta-sheet crystals provides mechanical strength and controllable biodegradation, while tropoelastin, a noncrystallizable elastic protein provides elasticity. Differential scanning calorimetry (DSC) and temperature modulated DSC (TMDSC) indicated that silk becomes miscible with tropoelastin at different blend ratios, without macrophase separation. Fourier transform infrared spectroscopy (FTIR) revealed secondary structural changes of the blend system (beta-sheet content) before and after methanol treatment. Atomic Force Microscopy (AFM) nano-indentation demonstrated that blending silk and tropoelastin at different ratios resulted in modification of mechanical features, with resilience from ~68% to ~97%, and elastic modulus between 2~9Mpa, depending on the ratio of the two polymers. Some of these values are close to those of native aortic elastin or elastin-like polypeptides. Significantly, during blending and drying silk-tropoelastin form micro- and nano-scale porous morphologies which promote human mesenchymal stem cell attachment and proliferation. These blends offer a new protein biomaterial system for cell support and tailored biomaterial properties to match mechanical needs. PMID:20674969

Invited review the coiled coil silk of bees, ants, and hornets.

Science.gov (United States)

Sutherland, Tara D; Weisman, Sarah; Walker, Andrew A; Mudie, Stephen T

2012-06-01

In this article, we review current knowledge about the silk produced by the larvae of bees, ants, and hornets [Apoidea and Vespoidea: Hymenoptera]. Different species use the silk either alone or in composites for a variety of purposes including mechanical reinforcement, thermal regulation, or humidification. The characteristic molecular structure of this silk is α-helical proteins assembled into tetrameric coiled coils. Gene sequences from seven species are available, and each species possesses a copy of each of four related silk genes that encode proteins predicted to form coiled coils. The proteins are ordered at multiple length scales within the labial gland of the final larval instar before spinning. The insects control the morphology of the silk during spinning to produce either fibers or sheets. The silk proteins are small and non repetitive and have been produced artificially at high levels by fermentation in E. coli. The artificial silk proteins can be fabricated into materials with structural and mechanical properties similar to those of native silks. Copyright © 2011 Wiley Periodicals, Inc.

Introducing biomimetic shear and ion gradients to microfluidic spinning improves silk fiber strength.

Science.gov (United States)

Li, David; Jacobsen, Matthew M; Gyune Rim, Nae; Backman, Daniel; Kaplan, David L; Wong, Joyce Y

2017-05-31

Silkworm silk is an attractive biopolymer for biomedical applications due to its high mechanical strength and biocompatibility; as a result, there is increasing interest in scalable devices to spin silk and recombinant silk so as to improve and customize their properties for diverse biomedical purposes (Vepari and Kaplan 2007 Prog. Polym. Sci. 32 ). While artificial spinning of regenerated silk fibroins adds tunability to properties such as degradation rate and surface functionalization, the resulting fibers do not yet approach the mechanical strength of native silkworm silk. These drawbacks reduce the applicability and attractiveness of artificial silk (Kinahan et al 2011 Biomacromolecules 12 ). Here, we used computational fluid dynamic simulations to incorporate shear in tandem with biomimetic ion gradients by coupling a modular novel glass microfluidic device to our previous co-axial flow device. Fibers spun with this combined apparatus demonstrated a significant increase in mechanical strength compared to fibers spun with the basic apparatus alone, with a three-fold increase in Young's modulus and extensibility and a twelve-fold increase in toughness. These results thus demonstrate the critical importance of ionic milieu and shear stress in spinning strong fibers from solubilized silk fibroin.

Poly(vinyl alcohol)-Tannic Acid Hydrogels with Excellent Mechanical Properties and Shape Memory Behaviors.

Science.gov (United States)

Chen, Ya-Nan; Peng, Lufang; Liu, Tianqi; Wang, Yaxin; Shi, Shengjie; Wang, Huiliang

2016-10-12

Shape memory hydrogels have promising applications in a wide variety of fields. Here we report the facile fabrication of a novel type of shape memory hydrogels physically cross-linked with both stronger and weaker hydrogen bonding (H-bonding). Strong multiple H-bonding formed between poly(vinyl alcohol) (PVA) and tannic acid (TA) leads to their coagulation when they are physically mixed at an elevated temperature and easy gelation at room temperature. The amorphous structure and strong H-bonding endow the PVA-TA hydrogels with excellent mechanical properties, as indicated by their high tensile strengths (up to 2.88 MPa) and high elongations (up to 1100%). The stronger H-bonding between PVA and TA functions as the "permanent" cross-link and the weaker H-bonding between PVA chains as the "temporary" cross-link. The reversible breakage and formation of the weaker H-bonding imparts the PVA-TA hydrogels with excellent temperature-responsive shape memory. Wet and dried hydrogel samples with a deformed or elongated shape can recover to their original shapes when immersed in 60 °C water in a few seconds or at 125 °C in about 2.5 min, respectively.

Beneficial Effects of Corn Silk on Metabolic Syndrome.

Science.gov (United States)

Wang, Bing; Xiao, Tiegang; Ruan, Jun; Liu, Wensheng

2017-01-01

Metabolic syndrome (MS) is a very common medical problem worldwide. It includes obesity, hypertension, hyperglycemia, and abnormal levels of triglycerides and high-density lipoprotein cholesterol. It is closely associated with insulin resistance and may lead to diabetes mellitus, liver diseases, or cardiovascular diseases. Corn silk (CS), a traditional Chinese medicine, has been reported to have multiple beneficial effects, including hypotensive, anti-diabetic, and hypolipidemic properties. This suggests that corn silk could be used to treat or prevent metabolic syndrome. In this review, we will discuss the potential role of corn silk in different components of metabolic syndrome. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

Mechanical properties and in vitro characterization of polyvinyl alcohol-nano-silver hydrogel wound dressings.

Science.gov (United States)

Oliveira, R N; Rouzé, R; Quilty, B; Alves, G G; Soares, G D A; Thiré, R M S M; McGuinness, G B

2014-02-06

Polyvinyl alcohol (PVA) hydrogels are materials for potential use in burn healing. Silver nanoparticles can be synthesized within PVA hydrogels giving antimicrobial hydrogels. Hydrogels have to be swollen prior to their application, and the common medium available for that in hospitals is saline solution, but the hydrogel could also take up some of the wound's fluid. This work developed gamma-irradiated PVA/nano-Ag hydrogels for potential use in burn dressing applications. Silver nitrate (AgNO3) was used as nano-Ag precursor agent. Saline solution, phosphate-buffered solution (PBS) pH 7.4 and solution pH 4.0 were used as swelling media. Microstructural evaluation revealed an effect of the nanoparticles on PVA crystallization. The swelling of the PVA-Ag samples in solution pH 4.0 was low, as was their silver delivery, compared with the equivalent samples swollen in the other media. The highest swelling and silver delivery were related to samples prepared with 0.50% AgNO3, and they also presented lower strength in PBS pH 7.4 and solution pH 4.0. Both PVA-Ag samples were also non-toxic and presented antimicrobial activity, confirming that 0.25% AgNO3 concentration is sufficient to establish an antimicrobial effect. Both PVA-Ag samples presented suitable mechanical and swelling properties in all media, representative of potential burn site conditions.

Photocrosslinked PLA-PEO-PLA Hydrogels from Self-Assembled Physical Networks: Mechanical Properties and Influence of Assumed Constitutive Relationships

Science.gov (United States)

Sanabria-DeLong, Naomi; Crosby, Alfred J.; Tew, Gregory N.

2014-01-01

Poly(lactide) – block – poly(ethylene oxide) – block – poly(lactide) [PLA-PEO-PLA] triblock copolymers are known to form physical hydrogels in water, due to the polymer's amphiphilicity. Their mechanical properties, biocompatibility, and biodegradability have made them attractive for use as soft tissue scaffolds. However, the network junction points are not covalently crosslinked and in a highly aqueous environment these hydrogels adsorb more water, transform from gel to sol, and lose the designed mechanical properties. In this report, a hydrogel was formed by using a novel two step approach. In the first step end-functionalized PLA-PEOPLA triblock was self-assembled into a physical hydrogel through hydrophobic micelle network junctions, and then, in the second step, this self-assembled physical network structure was locked into place by photocrosslinking the terminal acrylate groups. In contrast to physical hydrogels, the photocrosslinked gels remained intact in phosphate buffered solution at body temperature. The swelling, degradation, and mechanical properties were characterized and demonstrated extended degradation time (~ 65 days), exponential decrease in modulus with degradation time, and tunable shear modulus (1.6 – 133 kPa) by varying concentration. We also discuss the various constitutive relationships (Hookean, Neo-Hookean, and Mooney-Rivlin) that can be used to describe the stress-strain behavior of these hydrogels. The chosen model and assumptions used for data fitting influences the obtained modulus values by as much as a factor of 3.5, demonstrating the importance of clearly stating one's data fitting parameters so that accurate comparisons can be made within the literature. PMID:18817440

Study of the contribution of the state of water to the gel properties of a photocrosslinked polyacrylic acid hydrogel using magnetic resonance imaging.

Science.gov (United States)

Onuki, Yoshinori; Hasegawa, Naoki; Kida, Chihiro; Obata, Yasuko; Takayama, Kozo

2014-11-01

Photocrosslinked polyacrylic acid (PAA-HEMA) hydrogels are a promising candidate for use in dermatological patch adhesives. To gain further knowledge about the properties of this gel, we investigated the T1 relaxation time and the diffusion coefficient (D) of water in the hydrogels using magnetic resonance (MR) imaging. Hydrogels with different formulations and process factors were prepared and tested. The observed data were analyzed by ANOVA, which clarified the mode of action of the formulation and process factors based on these MR parameters. Various gel properties (i.e., gel fraction, swelling capacity, gel strength, and water-retention ability) were also measured, followed by a Bayesian network (BN) analysis. The BN allowed us to summarize well the relationships between the formulation and process factors, MR parameters, and gel properties. T1 was associated with the swelling and water-retention properties of the hydrogel, whereas D was associated with gel formation and gel strength. Furthermore, this study clarified that T1 and D mostly represented the hydration and water-compartmentalization effects of the hydrogel, respectively. In conclusion, the state of water seems to play an important role in the properties of the PAA-HEMA hydrogel. © 2014 Wiley Periodicals, Inc. and the American Pharmacists Association.

Natural fibers for hydrogels production and their applications in agriculture

Directory of Open Access Journals (Sweden)

Liliana Serna Cock

2017-10-01

Full Text Available This paper presents a review on hydrogels applied to agriculture emphasizing on the use of natural fibers. The objectives were to examine, trends in research addressed to identify natural fibers used in hydrogels development and methods for modifying natural fibers, understand factors which determine the water retention capacity of a hydrogel. Consequently, this paper shows some methodologies used to evaluate the hydrogels efficiency and to collect in tables, relevant information in relation to methods of natural fibers modification and hydrogel synthesis. It was found that previous research focused on hydrogels development processed with biodegradable polymers such as starch, chitosan and modified natural fibers, cross-linked with potassium acrylate and acrylamide, respectively. In addition, current researches aimed to obtaining hydrogels with improved properties, which have allowed a resistance to climatic variations and soil physicochemical changes, such as pH, presence of salts, temperature and composition. In fact, natural fibers such as sugarcane, agave fiber and kapok fiber, modified with maleic anhydride, are an alternative to obtain hydrogels due to an increasing of mechanical properties and chemically active sites. However, the use of natural nanofibers in hydrogels, has been a successful proposal to improve hydrogels mechanical and swelling properties, since they give to material an elasticity and rigidity properties. A hydrogel efficiency applied to soil, is measured throughout properties as swellability, mechanical strength, and soil water retention. It was concluded that hydrogels, are an alternative to the current needs for the agricultural sector.

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

Science.gov (United States)

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.

Graphene oxide from silk cocoon: a novel magnetic fluorophore for multi-photon imaging.

Science.gov (United States)

Roy, Manas; Kusurkar, Tejas Sanjeev; Maurya, Sandeep Kumar; Meena, Sunil Kumar; Singh, Sushil Kumar; Sethy, Niroj; Bhargava, Kalpana; Sharma, Raj Kishore; Goswami, Debabrata; Sarkar, Sabyasachi; Das, Mainak

2014-02-01

In this work, we synthesized graphene oxide from silk cocoon embarking its new dimension as a magnetic fluorophore when compared with its present technical status, which at best is for extracting silk as a biomaterial for tissue engineering applications. We produced graphene oxide by pyrolysing the silk cocoon in an inert atmosphere. The collected raw carbon is oxidized by nitric acid that readily produces multilayer graphene oxide with nano carbon particulates. Structural properties of the graphene oxide were analyzed using scanning electron microscopy, transmission electron microscopy, Fourier transform infra-red spectroscopy, and Raman spectroscopy. The oxidized sample shows remarkable fluorescence, multi-photon imaging and magnetic properties. On increasing the excitation wavelength, the fluorescence emission intensity of the graphene oxide also increases and found maximum emission at 380 nm excitation wavelength. On studying the two photon absorption (TPA) property of aqueous graphene oxide using Z-scan technique, we found significant TPA activity at near infrared wavelength. In addition, the graphene oxide shows ferromagnetic behavior at room temperature. The observed fluorescence and magnetic property were attributed to the defects caused in the graphene oxide structure by introducing oxygen containing hydrophilic groups during the oxidation process. Previously silk cocoon has been used extensively in deriving silk-based tissue engineering materials and as gas filter. Here we show a novel application of silk cocoon by synthesizing graphene oxide based magnetic-fluorophore for bio-imaging applications.

Radiation synthesis and characterization of thermo-sensitive PNIPA/clay hydrogels

International Nuclear Information System (INIS)

Song Hongyan; He Suqin; Liu Wentao; Zhu Chengshen; Yang Mingcheng

2007-01-01

In this work, the thermo-sensitive hydrogels of PNIPA/Clay were synthesized by 60 Co-γ rays irradiation. The effects of organically modified clay and Na + clay, clay content, and dispersing condition on swelling behavior of PNIPA/clay hydrogels were investigated. The results showed that the equilibrium swelling ratio (SR) of the PNIPA/clay hydrogels is better than PNIPA, and the SR of PNIPA/organically modified clay hydrogels is the highest. With clay content increases, the SR of hydrogels became better. The deswelling behavior of hydrogel was improved, the deswelling ratio of the hydrogel with organically modified clay is highest, and ratio of losing water is 83%, while PNIPA is about 50%. The compressive properties of hydrogel composites were also examined. The results showed that the compressive properties of the PNIPA/clay hydrogels were improved distinctly than that of the conventional hydrogels without clay. And with increasing of clay content, the compressive properties of hydrogel composites improve rapidly. When the content of clay is 15%, the maximum compression force of the PNIPA/clay hydrogel is 5.28N, which is 14 times of PNIPA hydrogel and compression strength is 2.5 times. (authors)

WOOD HEMICELLULOSE/CHITOSAN-BASED SEMI-INTERPENETRATING NETWORK HYDROGELS: MECHANICAL, SWELLING AND CONTROLLED DRUG RELEASE PROPERTIES

Directory of Open Access Journals (Sweden)

Muzaffer Ahmet Karaaslan

2010-04-01

Full Text Available The cell wall of most plant biomass from forest and agricultural resources consists of three major polymers, cellulose, hemicellulose, and lignin. Of these, hemicelluloses have gained increasing attention as sustainable raw materials. In this study, novel pH-sensitive semi-IPN hydrogels based on hemicelluloses and chitosan were prepared using glutaraldehyde as the crosslinking agent. The hemicellulose isolated from aspen was analyzed for sugar content by HPLC, and its molecular weight distribution was determined by high performance size exclusion chromatography. Results revealed that hemicellulose had a broad molecular weight distribution with a fair amount of polymeric units, together with xylose, arabinose, and glucose. The effects of hemicellulose content on mechanical properties and swelling behavior of hydrogels were investigated. The semi-IPNs hydrogel structure was confirmed by FT-IR, X-ray study, and the ninhydrin assay method. X-ray analysis showed that higher hemicellulose contents yielded higher crystallinity. Mechanical properties were mainly dependent on the crosslink density and average molecular weight between crosslinks. Swelling ratios increased with increasing hemicellulose content and were high at low pH values due to repulsion between similarly charged groups. In vitro release study of a model drug showed that these semi-IPN hydrogels could be used for controlled drug delivery into gastric fluid.

Self-assembly of silk fibroin under osmotic stress

Science.gov (United States)

Sohn, Sungkyun

The supramolecular self-assembly behavior of silk fibroin was investigated using osmotic stress technique. In Chapter 2, a ternary phase diagram of water-silk-LiBr was constructed based on X-ray results on the osmotically stressed regenerated silk fibroin of Bombyx mori silkworm. Microscopic data indicated that silk I is a hydrated structure and a rough estimate of the number of water molecules lost by the structure upon converting from silk I to silk II has been made, and found to be about 2.2 per [GAGAGS] hexapeptide. In Chapter 3, wet-spinning of osmotically stressed, regenerated silk fibroin was performed, based on the prediction that the enhanced control over structure and phase behavior using osmotic stress method helps improve the physical properties of wet-spun regenerated silk fibroin fibers. The osmotic stress was applied in order to pre-structure the regenerated silk fibroin molecule from its original random coil state to more oriented state, manipulating the phase of the silk solution in the phase diagram before the start of spinning. Monofilament fiber with a diameter of 20 microm was produced. In Chapter 4, we investigated if there is a noticeable synergistic osmotic pressure increase between co-existing polymeric osmolyte and salt when extremely highly concentrated salt molecules are present both at sample subphase and stressing subphase, as is the case of silk fibroin self-assembly. The equilibration method that measures osmotic pressure relative to a reference with known osmotic pressure was introduced. Osmotic pressure of aqueous LiBr solution up to 2.75M was measured and it was found that the synergistic effect was insignificant up to this salt concentration. Solution parameters of stressing solutions and Arrhenius kinetics based on time-temperature relationship for the equilibration process were derived as well. In Chapter 5, self-assembly behavior of natural silk fibroin within the gland of Bombyx mori silkworm was investigated using osmotic

Poly(AAc-co-MBA) hydrogel films: adhesive and mechanical properties in aqueous medium.

Science.gov (United States)

Arunbabu, Dhamodaran; Shahsavan, Hamed; Zhang, Wei; Zhao, Boxin

2013-01-10

Poly(acrylic acid-co-N,N'-methylenebisacrylamide) hydrogel films were synthesized by copolymerizing acrylic acid (AAc) with N,N'-methylenebisacrylamide (MBA) as a cross-linker via photo polymerization in the spacing confined between two glass plates. NMR spectroscopy was utilized to determine the cross-linking density. We found that the cross-linking density determined by NMR is higher than that expected from the feed concentrations of cross-linkers, suggesting that MBA is more reactive than AAc and the heterogeneous nature of the cross-linking. In addition to the swelling tests, indentation tests were performed on the hydrogel films under water to investigate effects of the cross-linking density on the adhesion and mechanical properties of the hydrogel films in terms of adhesive pull-off force and Hertz-type elastic modulus. As the cross-linker concentration increased, the effective elastic modulus of the hydrogel films increased dramatically at low cross-linking densities and reached a high steady-state value at higher cross-linking densities. The pull-off force decreased with increasing cross-linker concentration and reached a lower force plateau at high cross-linking densities. An optimal "trade-off" cross-linking density was determined to be 0.02 mol fraction of MBA in the hydrogel, where balanced elastic modulus and adhesive pull-off force can be obtained.

More than a safety line: jump-stabilizing silk of salticids.

Science.gov (United States)

Chen, Yung-Kang; Liao, Chen-Pan; Tsai, Feng-Yueh; Chi, Kai-Jung

2013-10-06

Salticids are diurnal hunters known for acute vision, remarkable predatory strategies and jumping ability. Like other jumpers, they strive for stability and smooth landings. Instead of using inertia from swinging appendages or aerodynamic forces by flapping wings as in other organisms, we show that salticids use a different mechanism for in-air stability by using dragline silk, which was previously believed to function solely as a safety line. Analyses from high-speed images of jumps by the salticid Hasarius adansoni demonstrate that despite being subject to rearward pitch at take-off, spiders with dragline silk can change body orientation in the air. Instantaneous drag and silk forces calculated from kinematic data further suggest a comparable contribution to deceleration and energy dissipation, and reveal that adjustments by the spider to the silk force can reverse its body pitch for a predictable and optimal landing. Without silk, upright-landing spiders would slip or even tumble, deferring completion of landing. Thus, for salticids, dragline silk is critical for dynamic stability and prey-capture efficiency. The dynamic functioning of dragline silk revealed in this study can advance the understanding of silk's physiological control over material properties and its significance to spider ecology and evolution, and also provide inspiration for future manoeuvrable robot designs.

Bioinspired Nanocomposite Hydrogels with Highly Ordered Structures.

Science.gov (United States)

Zhao, Ziguang; Fang, Ruochen; Rong, Qinfeng; Liu, Mingjie

2017-12-01

In the human body, many soft tissues with hierarchically ordered composite structures, such as cartilage, skeletal muscle, the corneas, and blood vessels, exhibit highly anisotropic mechanical strength and functionality to adapt to complex environments. In artificial soft materials, hydrogels are analogous to these biological soft tissues due to their "soft and wet" properties, their biocompatibility, and their elastic performance. However, conventional hydrogel materials with unordered homogeneous structures inevitably lack high mechanical properties and anisotropic functional performances; thus, their further application is limited. Inspired by biological soft tissues with well-ordered structures, researchers have increasingly investigated highly ordered nanocomposite hydrogels as functional biological engineering soft materials with unique mechanical, optical, and biological properties. These hydrogels incorporate long-range ordered nanocomposite structures within hydrogel network matrixes. Here, the critical design criteria and the state-of-the-art fabrication strategies of nanocomposite hydrogels with highly ordered structures are systemically reviewed. Then, recent progress in applications in the fields of soft actuators, tissue engineering, and sensors is highlighted. The future development and prospective application of highly ordered nanocomposite hydrogels are also discussed. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

3D printing of an interpenetrating network hydrogel material with tunable viscoelastic properties.

Science.gov (United States)

Bootsma, Katherine; Fitzgerald, Martha M; Free, Brandon; Dimbath, Elizabeth; Conjerti, Joe; Reese, Greg; Konkolewicz, Dominik; Berberich, Jason A; Sparks, Jessica L

2017-06-01

Interpenetrating network (IPN) hydrogel materials are recognized for their unique mechanical properties. While IPN elasticity and toughness properties have been explored in previous studies, the factors that impact the time-dependent stress relaxation behavior of IPN materials are not well understood. Time-dependent (i.e. viscoelastic) mechanical behavior is a critical design parameter in the development of materials for a variety of applications, such as medical simulation devices, flexible substrate materials, cellular mechanobiology substrates, or regenerative medicine applications. This study reports a novel technique for 3D printing alginate-polyacrylamide IPN gels with tunable elastic and viscoelastic properties. The viscoelastic stress relaxation behavior of the 3D printed alginate-polyacrylamide IPN hydrogels was influenced most strongly by varying the concentration of the acrylamide cross-linker (MBAA), while the elastic modulus was affected most by varying the concentration of total monomer material. The material properties of our 3D printed IPN constructs were consistent with those reported in the biomechanics literature for soft tissues such as skeletal muscle, cardiac muscle, skin and subcutaneous tissue. Copyright © 2017 Elsevier Ltd. All rights reserved.

Swelling and Shrinking Properties of Thermo-Responsive Polymeric Ionic Liquid Hydrogels with Embedded Linear pNIPAAM

Directory of Open Access Journals (Sweden)

Simon Gallagher

2014-03-01

Full Text Available In this study, varying concentrations of linear pNIPAAM have been incorporated for the first time into a thermo-responsive polymeric ionic liquid (PIL hydrogel, namely tributyl-hexyl phosphonium 3-sulfopropylacrylate (P-SPA, to produce semi-interpenetrating polymer networks. The thermal properties of the resulting hydrogels have been investigated along with their thermo-induced shrinking and reswelling capabilities. The semi-interpenetrating networks (IPN hydrogels were found to have improved shrinking and reswelling properties compared with their PIL counterpart. At elevated temperatures (50–80 °C, it was found that the semi-IPN with the highest concentration of hydrophobic pNIPAAM exhibited the highest shrinking percentage of ~40% compared to the conventional P-SPA, (27%. This trend was also found to occur for the reswelling measurements, with semi-IPN hydrogels producing the highest reswelling percentage of ~67%, with respect to its contracted state. This was attributed to an increase in water affinity due to the presence of hydrophilic pNIPAAM. Moreover, the presence of linear pNIPAAM in the polymer matrix leads to improved shrinking and reswelling response compared to the equivalent PIL.

Development of sago starch hydrogel for wound dressing

Energy Technology Data Exchange (ETDEWEB)

Kamaruddin Hashim; Khairul Zaman HJ. Mohd Dahlan; Kamarudin Bahari [Malaysian Institute for Nuclear Technology Research (MINT), Bangi (Malaysia); Yoshii, Fumio; Kume, Tamikazu [Japan Atomic Energy Research Inst., Takasaki, Gunma (Japan). Takasaki Radiation Chemistry Research Establishment

2001-03-01

Sago starch is utilized in Malaysia mainly for food production. The purpose of the research is to diversify the use of sago starch for medical application particularly in development of hydrogel burn wound dressing. The sago starch is blending with mixture of PVP and PVA to improve the degree of crosslink, mechanical properties, swelling ability and tackiness of the blend hydrogel (sago/PVA and sago PVP). Additives have been introduced into the system such as, polypropylene glycol or carboxymethyl cellulose to improved further the swelling ability and tackiness properties of the blend hydrogel as well as other properties. Effect of irradiation dose on the blend hydrogel has also been studied to optimize the effective dose for blend hydrogel and simultaneously for sterilization purpose. (author)

Development of sago starch hydrogel for wound dressing

International Nuclear Information System (INIS)

Kamaruddin Hashim; Khairul Zaman HJ Mohd Dahlan; Kamarudin Bahari; Yoshii, Fumio; Kume, Tamikazu

2001-01-01

Sago starch is utilized in Malaysia mainly for food production. The purpose of the research is to diversify the use of sago starch for medical application particularly in development of hydrogel burn wound dressing. The sago starch is blending with mixture of PVP and PVA to improve the degree of crosslink, mechanical properties, swelling ability and tackiness of the blend hydrogel (sago/PVA and sago PVP). Additives have been introduced into the system such as, polypropylene glycol or carboxymethyl cellulose to improved further the swelling ability and tackiness properties of the blend hydrogel as well as other properties. Effect of irradiation dose on the blend hydrogel has also been studied to optimize the effective dose for blend hydrogel and simultaneously for sterilization purpose. (author)

Formulation and release of alaptide from cellulose-based hydrogels

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Zbyněk Sklenář

2012-01-01

Full Text Available The modern drug alaptide, synthetic dipeptide, shows regenerative effects and effects on the epitelisation process. A commercial product consisting of 1% alaptide hydrophilic cream is authorised for use in veterinary practice. This study focuses on the formulation of alaptide into semi-synthetic polymer-based hydrogels. The aim of the present study is to prepare hydrogels and to evaluate the liberation of alaptide from hydrogels. The hydrogels were prepared on the basis of three gel-producing substances: methylcellulose, hydroxyethylcellulose and hydroxypropylcellulose. To enhance the drug release from hydrogel humectants, glycerol, propylene glycol and ethanol in various concentrations were evaluated. The permeation of the alaptide from gels into the acceptor solution was evaluated with the use of the permeable membrane neprophane. The amount of drug released from prepared hydrogels was determined spectrophotometrically. Hydrogels with optimal alaptide liberation properties were subjected to the study of rheological properties in the next phase. The optimal composition of hydrogel as established in this study was 1% alaptide + 3% hydroxyethylcellulose with the addition of 10% glycerol as humectant. Due to the advantageous properties of hydrogels in wounds, alaptide could be incorporated into a hydrogel base for use in veterinary medicine.

Gel spinning of silk tubes for tissue engineering

Science.gov (United States)

Lovett, Michael; Cannizzaro, Christopher; Vunjak-Novakovic, Gordana; Kaplan, David L.

2011-01-01

Tubular vessels for tissue engineering are typically fabricated using a molding, dipping, or electrospinning technique. While these techniques provide some control over inner and outer diameters of the tube, they lack the ability to align the polymers or fibers of interest throughout the tube. This is an important aspect of biomaterial composite structure and function for mechanical and biological impact of tissue outcomes. We present a novel aqueous process system to spin tubes from biopolymers and proteins such as silk fibroin. Using silk as an example, this method of winding an aqueous solution around a reciprocating rotating mandrel offers substantial improvement in the control of the tube properties, specifically with regard to winding pattern, tube porosity, and composite features. Silk tube properties are further controlled via different post-spinning processing mechanisms such as methanol-treatment, air-drying, and lyophilization. This approach to tubular scaffold manufacture offers numerous tissue engineering applications such as complex composite biomaterial matrices, blood vessel grafts and nerve guides, among others. PMID:18801570

Silk-Silk Interactions between Silkworm Fibroin and Recombinant Spider Silk Fusion Proteins Enable the Construction of Bioactive Materials.

Science.gov (United States)

Nilebäck, Linnea; Chouhan, Dimple; Jansson, Ronnie; Widhe, Mona; Mandal, Biman B; Hedhammar, My

2017-09-20

Natural silk is easily accessible from silkworms and can be processed into different formats suitable as biomaterials and cell culture matrixes. Recombinant DNA technology enables chemical-free functionalization of partial silk proteins through fusion with peptide motifs and protein domains, but this constitutes a less cost-effective production process. Herein, we show that natural silk fibroin (SF) can be used as a bulk material that can be top-coated with a thin layer of the recombinant spider silk protein 4RepCT in fusion with various bioactive motifs and domains. The coating process is based on a silk assembly to achieve stable interactions between the silk types under mild buffer conditions. The assembly process was studied in real time by quartz crystal microbalance with dissipation. Coatings, electrospun mats, and microporous scaffolds were constructed from Antheraea assama and Bombyx mori SFs. The morphology of the fibroin materials before and after coating with recombinant silk proteins was analyzed by scanning electron microscopy and atomic force microscopy. SF materials coated with various bioactive 4RepCT fusion proteins resulted in directed antibody capture, enzymatic activity, and improved cell attachment and spreading, respectively, compared to pristine SF materials. The herein-described procedure allows a fast and easy route for the construction of bioactive materials.

Effect of solvents on properties of Bombyx mori silk grafted by methyl methacrylate (MMA and methacrylamide (MAA

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Wattana Klairatsamee

2005-11-01

Full Text Available Mulberry silks were chemically modified in order to increase weight gain, resulting from degumming process using graft copolymerisation technique with vinyl monomers, i.e. MMA, MAA and MMA/MAA. Due to the appearance of PMMA homopolymer granules adhered on the MMA- and MMA/MAA-grafted silk surfaces resulting in surface roughness when silk was grafted by MMA in water, the influence of grafting solvents was examined, using different water/ethanol volume ratios of 100/0, 75/25, 50/50, 25/75 and 0/100. FTIR spectra of the grafted silks presented the absorption bands of the vinyl monomers used for the grafting process. In addition, high values of % polymer add-on were obtained for all of the grafted silks. It was also found that the suitable solvents were 25/75 water/ethanol for the silk grafted by MMA and MMA/MAA, and water for the silk grafted by MAA, in order to get the smooth grafted silk surface and high polymer add-on. Moreover, all the grafted silks showed slightly greater stiffness, as indicated by the increase of Young's modulus and the decrease of elongation.

Co-assembly of chitosan and phospholipids into hybrid hydrogels

DEFF Research Database (Denmark)

Mendes, Ana Carina Loureiro; Shekarforoush, Elhamalsadat; Engwer, Christoph

2016-01-01

Novel hybrid hydrogels were formed by adding chitosan (Ch) to phospholipids (P) self-assembled particles in lactic acid. The effect of the phospholipid concentration on the hydrogel properties was investigated and was observed to affect the rate of hydrogel formation and viscoelastic properties...

Formation of different gold nanostructures by silk nanofibrils

International Nuclear Information System (INIS)

Fang, Guangqiang; Yang, Yuhong; Yao, Jinrong; Shao, Zhengzhong; Chen, Xin

2016-01-01

Metal nanostructures that have unique size- and shape-dependent electronic, optical and chemical properties gain more and more attention in modern science and technology. In this article, we show the possibility that we are able to obtain different gold nanostructures simply with the help of silk nanofibrils. We demonstrate that only by varying the pH of the reaction solution, we get gold nanoparticles, nano-icosahedrons, nanocubes, and even microplates. Particularly, we develop a practical method for the preparation of gold microplates in acid condition in the presence of silk nanofibrils, which is impossible by using other forms of silk protein. We attribute the role of silk nanofibrils in the formation of gold nanostructure to their reduction ability from several specific amino acid residues, and the suitable structural anisotropic features to sustain the crystal growth after the reduction process. Although the main purpose of this article is to demonstrate that silk nanofibrils are able to mediate the formation of different gold nanostructure, we show the potential applications of these resulting gold nanostructures, such as surface-enhanced Raman scattering (SERS) and photothermal transformation effect, as same as those produced by other methods. In conclusion, we present in this communication a facile and green synthesis route to prepare various gold nanostructures with silk nanofibrils by simply varying pH in the reaction system, which has remarkable advantages in future biomedical applications. - Highlights: • Different Au nanostructures can be obtained by a facile and green protein reduction method. • Silk nanofibrils serve as both reductant and template in the formation of Au nanostructures. • Different Au nanostructures can be obtained simply by regulating the pH in the medium. • Large Au microplates can be obtained with a cheap, abundant, sustainable silk protein. • Silk/Au hybrid nanocomposites show potential application in SERS and

Formation of different gold nanostructures by silk nanofibrils

Energy Technology Data Exchange (ETDEWEB)

Fang, Guangqiang [State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Polymers and Polymer Composite Materials, Department of Macromolecular Science, Laboratory of Advanced Materials, Fudan University, Shanghai, 200433 (China); Yang, Yuhong [Research Centre for Analysis and Measurement, Fudan University, Shanghai 200433 (China); Yao, Jinrong; Shao, Zhengzhong [State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Polymers and Polymer Composite Materials, Department of Macromolecular Science, Laboratory of Advanced Materials, Fudan University, Shanghai, 200433 (China); Chen, Xin, E-mail: chenx@fudan.edu.cn [State Key Laboratory of Molecular Engineering of Polymers, Collaborative Innovation Center of Polymers and Polymer Composite Materials, Department of Macromolecular Science, Laboratory of Advanced Materials, Fudan University, Shanghai, 200433 (China)

2016-07-01

Metal nanostructures that have unique size- and shape-dependent electronic, optical and chemical properties gain more and more attention in modern science and technology. In this article, we show the possibility that we are able to obtain different gold nanostructures simply with the help of silk nanofibrils. We demonstrate that only by varying the pH of the reaction solution, we get gold nanoparticles, nano-icosahedrons, nanocubes, and even microplates. Particularly, we develop a practical method for the preparation of gold microplates in acid condition in the presence of silk nanofibrils, which is impossible by using other forms of silk protein. We attribute the role of silk nanofibrils in the formation of gold nanostructure to their reduction ability from several specific amino acid residues, and the suitable structural anisotropic features to sustain the crystal growth after the reduction process. Although the main purpose of this article is to demonstrate that silk nanofibrils are able to mediate the formation of different gold nanostructure, we show the potential applications of these resulting gold nanostructures, such as surface-enhanced Raman scattering (SERS) and photothermal transformation effect, as same as those produced by other methods. In conclusion, we present in this communication a facile and green synthesis route to prepare various gold nanostructures with silk nanofibrils by simply varying pH in the reaction system, which has remarkable advantages in future biomedical applications. - Highlights: • Different Au nanostructures can be obtained by a facile and green protein reduction method. • Silk nanofibrils serve as both reductant and template in the formation of Au nanostructures. • Different Au nanostructures can be obtained simply by regulating the pH in the medium. • Large Au microplates can be obtained with a cheap, abundant, sustainable silk protein. • Silk/Au hybrid nanocomposites show potential application in SERS and

Transient Dynamic Mechanical Analysis of Resilin-based Elastomeric Hydrogels

Science.gov (United States)

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 (engineering applications, of a range of RLP hydrogels.

Development and Evaluation of Isoniazid Loaded Silk Fibroin Microsphere

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Narinder Singh

Full Text Available Aim: Current experimental investigation is dedicated to prepare microspheres with small size and good sphericity by Phase Separation method using Isoniazid (INH as model drug. Silk fibroin has unique intrinsic qualities like biodegradability, biocompatibility or release properties and their tunable drug loading capacity. The delivery loading proficiency of the drug molecules in silk spheres be contingent on their charge, and hydrophobicity or subsequent in altered drug release profiles. Methods: In the present work Isoniazid loaded silk fibroin microsphere was prepared by using phase separation method. Microsphere was evaluated for Ultraviolet-visible spectroscopy, Fourier Transform infrared spectroscopy, Entrapment efficiency, Scanning electron microscopy Studies. Results: Scanning electron microscopy studies revealed that Isoniazid Loaded Silk Fibroin Microspheres were spherical. Entrapment Efficiency of Isoniazid loaded Microspheres of different Formulation from F1 to F5 was in range of 53 to 68 %. F3 showed 68.47 % entrapment Efficiency and the optimized formulation drug release was 93.56 % at 24 hours. Conclusion: Experimental report disclosed a new aqueous based formulation method for silk spheres with controllable shape or size and sphere. Isoniazid loaded silk microspheres may act as ideal nano formulation with elaborated studies.

Biomedical hydrogels biochemistry, manufacture and medical applications

CERN Document Server

Rimmer, Steve

2011-01-01

Hydrogels are very important for biomedical applications because they can be chemically manipulated to alter and control the hydrogel's interaction with cells and tissues. Their flexibility and high water content is similar to that of natural tissue, making them extremely suitable for biomaterials applications. Biomedical hydrogels explores the diverse range and use of hydrogels, focusing on processing methods and novel applications in the field of implants and prostheses. Part one of this book concentrates on the processing of hydrogels, covering hydrogel swelling behaviour, superabsorbent cellulose-based hydrogels and regulation of novel hydrogel products, as well as chapters focusing on the structure and properties of hydrogels and different fabrication technologies. Part two covers existing and novel applications of hydrogels, including chapters on spinal disc and cartilage replacement implants, hydrogels for ophthalmic prostheses and hydrogels for wound healing applications. The role of hydrogels in imag...

Radiation-chemical preparation of poly(vinyl alcohol) hydrogels

International Nuclear Information System (INIS)

Duflot, Anastasia V.; Kitaeva, Natalia K.; Duflot, Vladimir R.

2015-01-01

This work reports the usage of method of radiation-chemical synthesis to prepare cross-linked hydrogels from poly(vinyl alcohol) modified with glycidyl methacrylate. Synthesis kinetics of modified poly(vinyl alcohol) and properties of hydrogels were studied. The gel fraction, swelling, mechanical properties, and water content of the hydrogels were measured. It was found that gel fraction increases with increasing radiation dose, concentration of modified poly(vinyl alcohol), and reaches 60%. It was established by differential scanning calorimetry that a fraction of the “bound” water in hydrogels is 50–70% and independent of gel fraction content. In addition to “bound” and “free” states, water in hydrogels is also present in the intermediate state. - Highlights: • The synthesis and the properties of poly(vinyl alcohol) hydrogels were studied. • PVA was modified by glycidyl methacrylate before gamma cross-linking. • The modification results in decreasing of PVA cross-linking dose by 3 orders lower. • The gel fraction and water content of the hydrogels were measured. • A fraction of the “bound” water in hydrogels is independent of gel fraction content

Novel Hydrogels from Renewable Resources

Science.gov (United States)

Karaaslan, Muzafer Ahmet

2011-12-01

The cell wall of most plant biomass from forest and agricultural resources consists of three major polymers, cellulose, hemicellulose and lignin. Of these, hemicelluloses have gained increasing attention as sustainable raw materials. In the first part of this study, novel pH-sensitive semi-IPN hydrogels based on hemicelluloses and chitosan were prepared using glutaraldehyde as the crosslinking agent. The hemicellulose isolated from aspen was analyzed for sugar content by HPLC, and its molecular weight distribution was determined by high performance size exclusion chromatography. Results revealed that hemicellulose had a broad molecular weight distribution with a fair amount of polymeric units, together with xylose, arabinose and glucose. The effect of hemicellulose content on mechanical properties and swelling behavior of hydrogels were investigated. The semi-IPNs hydrogel structure was confirmed by FT-IR, X-ray study and ninhydrin assay method. X-ray analysis showed that higher hemicellulose contents yielded higher crystallinity. Mechanical properties were mainly dependent on the crosslink density and average molecular weight between crosslinks. Swelling ratios increased with increasing hemicellulose content and were high at low pH values due to repulsion between similarly charged groups. In vitro release study of a model drug showed that these semi-IPN hydrogels could be used for controlled drug delivery into gastric fluid. The aim of the second part of this study was to control the crosslink density and the mechanical properties of hemicellulose/chitosan semi-IPN hydrogels by changing the crosslinking sequence. It has been hypothesized that by performing the crosslinking step before introducing hemicellulose, covalent crosslinking of chitosan would not be hindered and therefore more and/or shorter crosslinks could be formed. Furthermore, additional secondary interactions and crystalline domains introduced through hemicellulose could be favorable in terms of

Tribological properties of PVA/PVP blend hydrogels against articular cartilage.

Science.gov (United States)

Kanca, Yusuf; Milner, Piers; Dini, Daniele; Amis, Andrew A

2018-02-01

This research investigated in-vitro tribological performance of the articulation of cartilage-on- polyvinyl alcohol (PVA) and polyvinyl pyrrolidone (PVP) blend hydrogels using a custom-designed multi-directional wear rig. The hydrogels were prepared by repeated freezing-thawing cycles at different concentrations and PVA to PVP fractions at a given concentration. PVA/PVP blend hydrogels showed low coefficient of friction (COF) values (between 0.12 ± 0.01 and 0.14 ± 0.02) which were closer to the cartilage-on-cartilage articulation (0.03 ± 0.01) compared to the cartilage-on-stainless steel articulation (0.46 ± 0.06). The COF increased with increasing hydrogel concentration (p = 0.03) and decreasing PVP content at a given concentration (p < 0.05). The cartilage-on-hydrogel tests showed only the surface layers of the cartilage being removed (average volume loss of the condyles was 12.5 ± 4.2mm 3 ). However, the hydrogels were found to be worn/deformed. The hydrogels prepared at a higher concentration showed lower apparent volume loss. A strong correlation (R 2 = 0.94) was found between the COF and compressive moduli of the hydrogel groups, resulting from decreasing contact congruency. It was concluded that the hydrogels were promising as hemiarthroplasty materials, but that improved mechanical behaviour was required for clinical use. Copyright © 2017 Elsevier Ltd. All rights reserved.

Bundles of spider silk, braided into sutures, resist basic cyclic tests: potential use for flexor tendon repair.

Directory of Open Access Journals (Sweden)

Kathleen Hennecke

Full Text Available Repair success for injuries to the flexor tendon in the hand is often limited by the in vivo behaviour of the suture used for repair. Common problems associated with the choice of suture material include increased risk of infection, foreign body reactions, and inappropriate mechanical responses, particularly decreases in mechanical properties over time. Improved suture materials are therefore needed. As high-performance materials with excellent tensile strength, spider silk fibres are an extremely promising candidate for use in surgical sutures. However, the mechanical behaviour of sutures comprised of individual silk fibres braided together has not been thoroughly investigated. In the present study, we characterise the maximum tensile strength, stress, strain, elastic modulus, and fatigue response of silk sutures produced using different braiding methods to investigate the influence of braiding on the tensile properties of the sutures. The mechanical properties of conventional surgical sutures are also characterised to assess whether silk offers any advantages over conventional suture materials. The results demonstrate that braiding single spider silk fibres together produces strong sutures with excellent fatigue behaviour; the braided silk sutures exhibited tensile strengths comparable to those of conventional sutures and no loss of strength over 1000 fatigue cycles. In addition, the braiding technique had a significant influence on the tensile properties of the braided silk sutures. These results suggest that braided spider silk could be suitable for use as sutures in flexor tendon repair, providing similar tensile behaviour and improved fatigue properties compared with conventional suture materials.

Mussel-inspired tough hydrogels with self-repairing and tissue adhesion

Science.gov (United States)

Gao, Zijian; Duan, Lijie; Yang, Yongqi; Hu, Wei; Gao, Guanghui

2018-01-01

The mussel-inspired polymeric hydrogels have been attractively explored owing to their self-repairing or adhesive property when the catechol groups of dopamine could chelate metal ions. However, it was a challenge for self-repairing hydrogels owning high mechanical properties. Herein, a synergistic strategy was proposed by combining catechol-Fe3+ complexes and hydrophobic association. The resulting hydrogels exhibited seamless self-repairing behavior, tissue adhesion and high mechanical property. Moreover, the pH-dependent stoichiometry of catechol-Fe3+ and temperature-sensitive hydrophobic association endue hydrogels with pH/thermo responsive characteristics. Subsequently, the self-repairing rate and mechanical property of hydrogels were investigated at different pH and temperature. This bio-inspired strategy would build an avenue for designing and constructing a new generation of self-repairing, tissue-adhesive and tough hydrogel.

Investigation of synthetic spider silk crystallinity and alignment via electrothermal, pyroelectric, literature XRD, and tensile techniques

NARCIS (Netherlands)

Munro, Troy; Putzeys, Tristan; Copeland, Cameron G.; Xing, Changhu; Lewis, Randolph V.; Ban, Heng; Glorieux, Christ; Wubbenhorst, Michael

2017-01-01

The processes used to create synthetic spider silk greatly affect the properties of the produced fibers. This paper investigates the effect of process variations during artificial spinning on the thermal and mechanical properties of the produced silk. Property values are also compared to the ones of

New application of silk protein

International Nuclear Information System (INIS)

Kamiishi, Youichi

2000-01-01

Gunma prefecture is famous for sericulture and silk textile industry district in Japan. In Gunma prefecture, some kinds of new generation silk as high performance and high quality silk were developed. These silk are used not only for the new textile materials but also for new industrial materials. New application of silk protein, fibroin and sericin, is considered. (author)

New application of silk protein

Energy Technology Data Exchange (ETDEWEB)

Kamiishi, Youichi [Textile Research Institute of Gunma, Kiryu, Gunma (Japan)

2000-03-01

Gunma prefecture is famous for sericulture and silk textile industry district in Japan. In Gunma prefecture, some kinds of new generation silk as high performance and high quality silk were developed. These silk are used not only for the new textile materials but also for new industrial materials. New application of silk protein, fibroin and sericin, is considered. (author)

Preparation and characterization of silk fibroin as a biomaterial with potential for drug delivery

Directory of Open Access Journals (Sweden)

Zhang Hao

2012-06-01

Full Text Available Abstract Background Degummed silk fibroin from Bombyx mori (silkworm has potential carrier capabilities for drug delivery in humans; however, the processing methods have yet to be comparatively analyzed to determine the differential effects on the silk protein properties, including crystalline structure and activity. Methods In this study, we treated degummed silk with four kinds of calcium-alcohol solutions, and performed secondary structure measurements and enzyme activity test to distinguish the differences between the regenerated fibroins and degummed silk fibroin. Results Gel electrophoresis analysis revealed that Ca(NO32-methanol, Ca(NO32-ethanol, or CaCl2-methanol treatments produced more lower molecular weights of silk fibroin than CaCl2-ethanol. X-ray diffraction and Fourier-transform infrared spectroscopy showed that CaCl2-ethanol produced a crystalline structure with more silk I (α-form, type II β-turn, while the other treatments produced more silk II (β-form, anti-parallel β-pleated sheet. Solid-State 13C cross polarization and magic angle spinning-nuclear magnetic resonance measurements suggested that regenerated fibroins from CaCl2-ethanol were nearly identical to degummed silk fibroin, while the other treatments produced fibroins with significantly different chemical shifts. Finally, enzyme activity test indicated that silk fibroins from CaCl2-ethanol had higher activity when linked to a known chemotherapeutic drug, L-asparaginase, than the fibroins from other treatments. Conclusions Collectively, these results suggest that the CaCl2-ethanol processing method produces silk fibroin with biomaterial properties that are appropriate for drug delivery.

Solubilization of spider silk proteins and its structural analysis using Fourier transform infrared spectroscopy

Science.gov (United States)

Osbin, K.; Jayan, Manuel; Bhadrakumari, S.; Predeep, P.

2017-06-01

This study investigates the presence of various amide bands present in different spider silk species, which provides extraordinary physical properties. Three different spider silks were collected from Western Ghats region. The collected spider silks samples belonging to the spider Heteropoda venatoria (species 1), Hersilia savignyi (species 2) and Pholcus phalangioides (species 3). Fourier transform infrared (FTIR) spectra reveals the protein peaks in the amide I, II, and III regions in all the three types of spider silk species.

Synthesis, characterization and properties of radiation-induced Starch/(EG-co-MAA hydrogels

Directory of Open Access Journals (Sweden)

H.L. Abd El-Mohdy

2016-11-01

Full Text Available Association of poly(carboxylic acids and non-ionic polymers in solutions via hydrogen bonding results in formation of novel polymeric materials–interpolymer complexes. Starch/(EG-co-MAA polymeric hydrogels were obtained by γ-initiated radiation copolymerization of ethylene glycol (EG with methacrylic acid (MAA which grafted on starch. The gel content of prepared hydrogels was varied with changes in starch content, EG:MAA composition and irradiation dose as well as crosslinking density. The swelling was studied as a function of starch content, EG:MAA composition, irradiation dose, type of soaked liquid, pH and temperature of matrix-surrounding medium. The degree of swelling greatly increased with enhanced MAA content, pH and temperature whereas, it decreased with reduced starch content and irradiation dose. The swelling was varied with the polarity of soaked liquid. The results showed that Starch/(EG-co-MAA hydrogels reached the equilibrium swelling state in water after 72 h. The structure and surface morphology of prepared polymer were confirmed with FTIR and SEM, respectively. The thermal properties of hydrogels were studied by using DSC and TGA, they cleared that there is miscibility between EG and MAA in copolymer and adding them improve the thermal stability of starch. The results indicate that Starch/(EG-co-MAA materials may be used in various applications.

Buyid Silk and the Tale of Bibi Shahrbanu: Identification of Biomarkers of Artificial Aging (Forgery) of Silk.

Science.gov (United States)

Moini, Mehdi; Rollman, Christopher M

2017-10-03

Buyid silk forgery is one of the most famous silk forgeries in the world. In 1924-1925, excavation of the Bibi Shahrbanu site in Iran unearthed several silk textiles. The silks were thought to be of the Buyid period (934-1062 BCE) of the Persian Empire and have since been known as the "Buyid silks". In the 1930s, more silk appeared and was reported as being from the Buyid period as well. Controversy over the authenticity of these silks escalated after the purchase of the silks by museums throughout the world. Extensive investigations of several of these silks have been conducted over the years with respect to iconography, weaving patterns, dyes/mordant, style, and even radiocarbon dating. It was found that most of the silks are not from Buyid period. To test the authenticity of these silk fabrics, the recently developed silk dating technique using amino acid racemization (AAR) in conjunction with capillary electrophoresis mass spectrometry was applied to 13 Buyid silk specimens from the Textile Museum collections. Among these silk specimens, the AAR ratios of only one specimen were consistent with authentic silk fabrics collected from various museums. In addition, the aspartic acid racemization ratio of this specimen was also consistent with its 14 C dating. The other "Buyid silks" showed excessive levels of amino acid racemization not only for aspartic acid, but also for phenylalanine and tyrosine, inconsistent with racemization rates of these amino acids in authentic historical silk fabrics. Treatment of modern silk with a base at different pH and temperature reproduced the AAR pattern of the Buyid silks, implying that chemical treatment with a base at relatively high temperatures was perhaps the method used to artificially age these fabrics. The results imply that the racemization ratios of aspartic acid, phenylalanine, and tyrosine can be used as biomarkers for identification of naturally versus artificially aged silk.

DNA preservation in silk.

Science.gov (United States)

Liu, Yawen; Zheng, Zhaozhu; Gong, He; Liu, Meng; Guo, Shaozhe; Li, Gang; Wang, Xiaoqin; Kaplan, David L

2017-06-27

The structure of DNA is susceptible to alterations at high temperature and on changing pH, irradiation and exposure to DNase. Options to protect and preserve DNA during storage are important for applications in genetic diagnosis, identity authentication, drug development and bioresearch. In the present study, the stability of total DNA purified from human dermal fibroblast cells, as well as that of plasmid DNA, was studied in silk protein materials. The DNA/silk mixtures were stabilized on filter paper (silk/DNA + filter) or filter paper pre-coated with silk and treated with methanol (silk/DNA + PT-filter) as a route to practical utility. After air-drying and water extraction, 50-70% of the DNA and silk could be retrieved and showed a single band on electrophoretic gels. 6% silk/DNA + PT-filter samples provided improved stability in comparison with 3% silk/DNA + filter samples and DNA + filter samples for DNA preservation, with ∼40% of the band intensity remaining at 37 °C after 40 days and ∼10% after exposure to UV light for 10 hours. Quantitative analysis using the PicoGreen assay confirmed the results. The use of Tris/borate/EDTA (TBE) buffer enhanced the preservation and/or extraction of the DNA. The DNA extracted after storage maintained integrity and function based on serving as a functional template for PCR amplification of the gene for zinc finger protein 750 (ZNF750) and for transgene expression of red fluorescence protein (dsRed) in HEK293 cells. The high molecular weight and high content of a crystalline beta-sheet structure formed on the coated surfaces likely accounted for the preservation effects observed for the silk/DNA + PT-filter samples. Although similar preservation effects were also obtained for lyophilized silk/DNA samples, the rapid and simple processing available with the silk-DNA-filter membrane system makes it appealing for future applications.

Effect of. gamma. -irradiation on the crystalline structure of silk fibroin and silk sericin

Energy Technology Data Exchange (ETDEWEB)

Tsukada, Masuhiro; Aoki, Akira

1985-02-01

Changes in the crystalline structure of silk sericin and silk fibroin induced by gamma-irradiation in the atmosphere described. The crystalline structure of silk sericin which had been subjected to gamma-irradiation remained unchanged. However the decomposition temperature of the specimen decreased to about 230 deg C, when the total dose of ..gamma.. rays exceeded 4.6 Mrad. The structure of the silk 1 type crystal of silk fibroin in the solid state, with a low degree of molecular orientation, changed into the silk 2 type crystal, when the total dose of ..gamma.. rays exceeded 4.6 Mrad. No changes in the crystalline structure were observed in the solid state of the silk 2 type crystal regardless of gamma-irradiation. The decrease in the decomposition temperature of the specimen was attributed to the decrease in the molecular orientation. However, the molecular conformation of silk fibroin with a randomly coiled structure remained unchanged even after gamma-irradiation.

Punctuated evolution of viscid silk in spider orb webs supported by mechanical behavior of wet cribellate silk

Science.gov (United States)

Piorkowski, Dakota; Blackledge, Todd A.

2017-08-01

The origin of viscid capture silk in orb webs, from cribellate silk-spinning ancestors, is a key innovation correlated with significant diversification of web-building spiders. Ancestral cribellate silk consists of dry nanofibrils surrounding a stiff, axial fiber that adheres to prey through van der Waals interactions, capillary forces, and physical entanglement. In contrast, viscid silk uses chemically adhesive aqueous glue coated onto a highly compliant and extensible flagelliform core silk. The extensibility of the flagelliform fiber accounts for half of the total work of adhesion for viscid silk and is enabled by water in the aqueous coating. Recent cDNA libraries revealed the expression of flagelliform silk proteins in cribellate orb-weaving spiders. We hypothesized that the presence of flagelliform proteins in cribellate silk could have allowed for a gradual shift in mechanical performance of cribellate axial silk, whose effect was masked by the dry nature of its adhesive. We measured supercontraction and mechanical performance of cribellate axial silk, in wet and dry states, for two species of cribellate orb web-weaving spiders to see if water enabled flagelliform silk-like performance. We found that compliance and extensibility of wet cribellate silk increased compared to dry state as expected. However, when compared to other silk types, the response to water was more similar to other web silks, like major and minor ampullate silk, than to viscid silk. These findings support the punctuated evolution of viscid silk mechanical performance.

Injectable self-healing carboxymethyl chitosan-zinc supramolecular hydrogels and their antibacterial activity.

Science.gov (United States)

Wahid, Fazli; Zhou, Ya-Ning; Wang, Hai-Song; Wan, Tong; Zhong, Cheng; Chu, Li-Qiang

2018-04-07

Injectable and self-healing hydrogels have found numerous applications in drug delivery, tissue engineering and 3D cell culture. Herein, we report an injectable self-healing carboxymethyl chitosan (CMCh) supramolecular hydrogels cross-linked by zinc ions (Zn 2+ ). Supramolecular hydrogels were obtained by simple addition of metal ions solution to CMCh solution at an appropriate pH value. The mechanical properties of these hydrogels were adjustable by the concentration of Zn 2+ . For example, the hydrogel with the highest concentration of Zn 2+ (CMCh-Zn4) showed strongest mechanical properties (storage modulus~11,000Pa) while hydrogel with the lowest concentration of Zn 2+ (CMCh-Zn1) showed weakest mechanical properties (storage modulus~220Pa). As observed visually and confirmed rheologically, the CMCh-Zn1 hydrogel with the lowest Zn 2+ concentration showed thixotropic property. CMCh-Zn1 hydrogel also presented injectable property. Moreover, the antibacterial properties of the prepared supramolecular hydrogels were studied against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) by agar well diffusion method. The results revealed Zn 2+ dependent antibacterial properties against both kinds of strains. The inhibition zones were ranging from ~11-24mm and ~10-22mm against S. aureus and E. coli, respectively. We believe that the prepared supramolecular hydrogels could be used as a potential candidate in biomedical fields. Copyright © 2018 Elsevier B.V. All rights reserved.

Arct'Alg release from hydrogel membranes

International Nuclear Information System (INIS)

Amaral, Renata H.; Rogero, Sizue O.; Shihomatsu, Helena M.; Lugao, Ademar B.

2009-01-01

The hydrogel properties make them attractive for a variety of biomedical and pharmaceutical applications, primarily in drug delivery system. Synthetic hydrogels have been studied to develop new devices for drugs or cosmetic active agents release. Arct'Alg R is an extract derived from red algae biomass which has antioxidant, anti-inflammatory and tissue regeneration stimulant properties. This extract was incorporated to poly(N-vinyl pyrrolidone) (PVP) and poly(vinyl alcohol) (PVA) hydrogel membranes obtained by gamma rays crosslinking technique. The ionizing radiation presents the advantage to occur polymerization and sterilization simultaneously in the same process. The aim of this work was the in vitro release kinetic study of Arct'Alg R from hydrogel membranes during 24 hours to verify the possibility of use in cosmetic and dermatological treatments. Results showed that about 50% and 30% of incorporated Arct'Alg R was released from PVP and PVA hydrogel membrane devices respectively. (author)

Effect of Sodium Carbonate Concentrations on the Formation and Mechanism of Regenerated Silk Fibroin Nanofibers by Electrospinning

Directory of Open Access Journals (Sweden)

Hao Dou

2014-01-01

Full Text Available Degumming is the first process for the preparation of all silk-based products. In this paper, effect of sodium carbonate concentrations for silk degumming on the formation of electrospun silk fibroin nanofibers was investigated and the reason for the silk electrospinning process was explained for the first time by differences from the microstructure of regenerated silk fibroin. With increasing the sodium carbonate concentration, microstructure both in the aqueous solutions and in the electrospinning solutions transformed from nanofibrils to nanoparticles, leading to obvious changes on rheological property; electrospinning solutions with nanofibrils behaved like the native silk dope and owned remarkably higher viscosity than the solutions with nanoparticles showing very low viscosity. More interestingly, nanofibrils favored the formation of silk nanofibers with ease, and even nanofibers could be electrospun at concentration 2%. However, nanoparticles were completely unable to generate nanofibers at high spinning concentration 8%. Importance of sodium carbonate concentrations is heavily emphasized for impacting the microstructure types and further influencing the electrospinning performance of regenerated silk. Hence, sodium carbonate concentrations provide a controllable choice for the preparation of silk-based electrospun biomaterials with desired properties.

Fluxgate magnetorelaxometry: a new approach to study the release properties of hydrogel cylinders and microspheres.

Science.gov (United States)

Wöhl-Bruhn, S; Heim, E; Schwoerer, A; Bertz, A; Harling, S; Menzel, H; Schilling, M; Ludwig, F; Bunjes, H

2012-10-15

Hydrogels are under investigation as long term delivery systems for biomacromolecules as active pharmaceutical ingredients. The release behavior of hydrogels can be tailored during the fabrication process. This study investigates the applicability of fluxgate magnetorelaxometry (MRX) as a tool to characterize the release properties of such long term drug delivery depots. MRX is based on the use of superparamagnetic core-shell nanoparticles as model substances. The feasibility of using superparamagnetic nanoparticles to study the degradation of and the associated release from hydrogel cylinders and hydrogel microspheres was a major point of interest. Gels prepared from two types of photo crosslinkable polymers based on modified hydroxyethylstarch, specifically hydroxyethyl starch-hydroxyethyl methacrylate (HES-HEMA) and hydroxyethyl starch-polyethylene glycol methacrylate (HES-P(EG)(6)MA), were analyzed. MRX analysis of the incorporated nanoparticles allowed to evaluate the influence of different crosslinking conditions during hydrogel production as well as to follow the increase in nanoparticle mobility as a result of hydrogel degradation during release studies. Conventional release studies with fluorescent markers (half-change method) were performed for comparison. MRX with superparamagnetic nanoparticles as model substances is a promising method to analyze pharmaceutically relevant processes such as the degradation of hydrogel drug carrier systems. In contrast to conventional release experiments MRX allows measurements in closed vials (reducing loss of sample and sampling errors), in opaque media and at low magnetic nanoparticle concentrations. Magnetic markers possess a better long-term stability than fluorescent ones and are thus also promising for the use in in vivo studies. Copyright © 2012 Elsevier B.V. All rights reserved.

Fabrication and characterization of biomaterial film from gland silk of muga and eri silkworms.

Science.gov (United States)

Dutta, Saranga; Talukdar, Bijit; Bharali, Rupjyoti; Rajkhowa, Rangam; Devi, Dipali

2013-05-01

This study discusses the possibilities of liquid silk (Silk gland silk) of Muga and Eri silk, the indigenous non mulberry silkworms of North Eastern region of India, as potential biomaterials. Silk protein fibroin of Bombyx mori, commonly known as mulberry silkworm, has been extensively studied as a versatile biomaterial. As properties of different silk-based biomaterials vary significantly, it is important to characterize the non mulberry silkworms also in this aspect. Fibroin was extracted from the posterior silk gland of full grown fifth instars larvae, and 2D film was fabricated using standard methods. The films were characterized using SEM, Dynamic contact angle test, FTIR, XRD, DSC, and TGA and compared with respective silk fibers. SEM images of films reveal presence of some globules and filamentous structure. Films of both the silkworms were found to be amorphous with random coil conformation, hydrophobic in nature, and resistant to organic solvents. Non mulberry silk films had higher thermal resistance than mulberry silk. Fibers were thermally more stable than the films. This study provides insight into the new arena of research in application of liquid silk of non mulberry silkworms as biomaterials. Copyright © 2012 Wiley Periodicals, Inc.

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

Science.gov (United States)

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.

A numerical model for ultrasonic measurements of swelling and mechanical properties of a swollen PVA hydrogel.

Science.gov (United States)

Lohakan, M; Jamnongkan, T; Pintavirooj, C; Kaewpirom, S; Boonsang, S

2010-08-01

This paper presents a numerical model for the evaluation of mechanical properties of a relatively thin hydrogel. The model utilizes a system identification method to evaluate the acoustical parameters from ultrasonic measurement data. The model involves the calculation of the forward model based on an ultrasonic wave propagation incorporating diffraction effect. Ultrasonic measurements of a hydrogel are also performed in a reflection mode. A Nonlinear Least Square (NLS) algorithm is employed to minimize difference between the results from the model and the experimental data. The acoustical parameters associated with the model are effectively modified to achieve the minimum error. As a result, the parameters of PVA hydrogels namely thickness, density, an ultrasonic attenuation coefficient and dispersion velocity are effectively determined. In order to validate the model, the conventional density measurements of hydrogels were also performed. Copyright (c) 2010 Elsevier B.V. All rights reserved.

Effects of the amino acid sequence on thermal conduction through β-sheet crystals of natural silk protein.

Science.gov (United States)

Zhang, Lin; Bai, Zhitong; Ban, Heng; Liu, Ling

2015-11-21

Recent experiments have discovered very different thermal conductivities between the spider silk and the silkworm silk. Decoding the molecular mechanisms underpinning the distinct thermal properties may guide the rational design of synthetic silk materials and other biomaterials for multifunctionality and tunable properties. However, such an understanding is lacking, mainly due to the complex structure and phonon physics associated with the silk materials. Here, using non-equilibrium molecular dynamics, we demonstrate that the amino acid sequence plays a key role in the thermal conduction process through β-sheets, essential building blocks of natural silks and a variety of other biomaterials. Three representative β-sheet types, i.e. poly-A, poly-(GA), and poly-G, are shown to have distinct structural features and phonon dynamics leading to different thermal conductivities. A fundamental understanding of the sequence effects may stimulate the design and engineering of polymers and biopolymers for desired thermal properties.

Structural Origins of Silk Piezoelectricity.

Science.gov (United States)

Yucel, Tuna; Cebe, Peggy; Kaplan, David L

2011-02-22

Uniaxially oriented, piezoelectric silk films were prepared by a two-step method that involved: (1) air drying aqueous, regenerated silk fibroin solutions into films, and (2) drawing the silk films to a desired draw ratio. The utility of two different drawing techniques, zone drawing and water immersion drawing were investigated for processing the silk for piezoelectric studies. Silk films zone drawn to a ratio of λ= 2.7 displayed relatively high dynamic shear piezoelectric coefficients of d(14) = -1.5 pC/N, corresponding to over two orders of magnitude increase in d(14) due to film drawing. A strong correlation was observed between the increase in the silk II, β-sheet content with increasing draw ratio measured by FTIR spectroscopy (C(β)∝ e(2.5) (λ)), the concomitant increasing degree of orientation of β-sheet crystals detected via WAXD (FWHM = 0.22° for λ= 2.7), and the improvement in silk piezoelectricity (d(14)∝ e(2.4) (λ)). Water immersion drawing led to a predominantly silk I structure with a low degree of orientation (FWHM = 75°) and a much weaker piezoelectric response compared to zone drawing. Similarly, increasing the β-sheet crystallinity without inducing crystal alignment, e.g. by methanol treatment, did not result in a significant enhancement of silk piezoelectricity. Overall, a combination of a high degree of silk II, β-sheet crystallinity and crystalline orientation are prerequisites for a strong piezoelectric effect in silk. Further understanding of the structural origins of silk piezoelectricity will provide important options for future biotechnological and biomedical applications of this protein.

Development of novel electrospun nanofibrous scaffold from P. ricini and A. mylitta silk fibroin blend with improved surface and biological properties

International Nuclear Information System (INIS)

Panda, N.; Bissoyi, A.; Pramanik, K.; Biswas, A.

2015-01-01

Biomaterials that stimulate cell attachment and proliferation without any surface modification (e.g. RGD coating) provide potent and cost effective scaffold for regenerative medicine. This study assessed the physico-chemical properties and cell supportive potential of a silk fibroin blend scaffold derived from eri (Philosamia ricini) and tasar (Antheraea mylitta) silk (ET) respectively by electrospinning process. The scanning electron microscopy and transmission electron microscopy study found that the fiber diameters are in 200 to 800 nm range with flat morphology. The porosity of ET scaffold is found to be 79 ± 5% with majority of pore diameter between 2.5 to 5 nm. Similarly, Bombyx mori (BM) silk fibroin and gelatin nanofibrous scaffolds were prepared and taken as control. The ultimate tensile strength of the ET and BM scaffold are found to be 1.83 ± 0.13 MPa and 1.47 ± 0.10 MPa respectively. The measured contact angle (a measure of hydrophilicity) for ET (54.7° ± 1.8°) is found to be lower than BM (62° ± 2.3°). The ability to deposit apatite over ET is comparable to that of BM nanofibers. All the scaffolds were seeded with cord blood derived mesenchymal stem cells (hMSCs) and cultured for 14 days in vitro. The immunofluorescence study reveals enhanced cell attachment with higher metabolic activity for MSCs grown over ET than BM and gelatin. The ET scaffold also demonstrated expression of higher amount cell adhesion molecules (CD29/CD44) and higher proliferation rate than BM and gelatin as confirmed by MTT assay, DNA content estimation assay, flow cytometry study and SEM study. Overall, it may be concluded that ET scaffold may have potential in developing bone tissue grafts for clinical applications in the future. - Highlights: • We have fabricated eri–tasar blended electrospun silk fibroin nanofiber with superior surface property. • The hydrophilicity is higher than the silk fibroin nanofiber derived from Bombyx mori (BM). • The nanofibrous

Development of novel electrospun nanofibrous scaffold from P. ricini and A. mylitta silk fibroin blend with improved surface and biological properties

Energy Technology Data Exchange (ETDEWEB)

Panda, N.; Bissoyi, A.; Pramanik, K.; Biswas, A., E-mail: amitb79@gmail.com

2015-03-01

Biomaterials that stimulate cell attachment and proliferation without any surface modification (e.g. RGD coating) provide potent and cost effective scaffold for regenerative medicine. This study assessed the physico-chemical properties and cell supportive potential of a silk fibroin blend scaffold derived from eri (Philosamia ricini) and tasar (Antheraea mylitta) silk (ET) respectively by electrospinning process. The scanning electron microscopy and transmission electron microscopy study found that the fiber diameters are in 200 to 800 nm range with flat morphology. The porosity of ET scaffold is found to be 79 ± 5% with majority of pore diameter between 2.5 to 5 nm. Similarly, Bombyx mori (BM) silk fibroin and gelatin nanofibrous scaffolds were prepared and taken as control. The ultimate tensile strength of the ET and BM scaffold are found to be 1.83 ± 0.13 MPa and 1.47 ± 0.10 MPa respectively. The measured contact angle (a measure of hydrophilicity) for ET (54.7° ± 1.8°) is found to be lower than BM (62° ± 2.3°). The ability to deposit apatite over ET is comparable to that of BM nanofibers. All the scaffolds were seeded with cord blood derived mesenchymal stem cells (hMSCs) and cultured for 14 days in vitro. The immunofluorescence study reveals enhanced cell attachment with higher metabolic activity for MSCs grown over ET than BM and gelatin. The ET scaffold also demonstrated expression of higher amount cell adhesion molecules (CD29/CD44) and higher proliferation rate than BM and gelatin as confirmed by MTT assay, DNA content estimation assay, flow cytometry study and SEM study. Overall, it may be concluded that ET scaffold may have potential in developing bone tissue grafts for clinical applications in the future. - Highlights: • We have fabricated eri–tasar blended electrospun silk fibroin nanofiber with superior surface property. • The hydrophilicity is higher than the silk fibroin nanofiber derived from Bombyx mori (BM). • The nanofibrous

Flame retardancy and ultraviolet resistance of silk fabric coated by graphene oxide

Directory of Open Access Journals (Sweden)

Ji Yi-Min

2017-01-01

Full Text Available Silk fabrics were coated by graphene oxide hydrosol in order to improve its flame retardancy and ultraviolet resistance. In addition, montmorillonoid was doped into the graphene oxide hydrosol to further improve the flame retardancy of silk fabrics. The flame retardancy and ultraviolet resistance were mainly characterized by limiting oxygen index, vertical flame test, smoke density test, and ultraviolet protection factor. The synergistic effect of graphene oxide and montmorillonoid on the thermal stabilization property of the treated silk fabrics was also investigated. The results show that the treated silk fabrics have excellent flame retardancy, thermal stability, smoke suppression, and ultraviolet resistance simultaneously.

Radiation-induced synthesis and swelling properties of p(2-hydroxyethyl methacrylate-co-itaconic acid-co-oligo(ethylene glycol) acrylate) copolymeric hydrogels

International Nuclear Information System (INIS)

Micic, M.; Suljovrujic, E.

2011-01-01

Complete text of publication follows. Since it is presumed that by incorporation of pH-responsive (IA) and temperature-responsive (OEGA) co-monomers it is possible to prepare P(HEMA-co-IA-co-OEGA) hydrogels with duel (pH and thermo) responsiveness, the main purpose of this paper is to investigate the influence of different mole fractions of IA and especially OEGA on the diversity of the swelling properties of obtained hydrogels. For that reason, a series of copolymeric hydrogels with different mole ratios of 2-hydroxyethyl methacrylate (HEMA), itaconic acid (IA) and oligo(ethylene glycol) acrylates (OEGA) was synthesized by gamma radiation. The obtained hydrogels were characterized by swelling studies in the wide pH (2.2-9.0) and temperature range (25-70 deg C), confirming dual (pH and thermo) responsiveness and a large variation in swelling capability. It was observed that the equilibrium swelling of P(HEMA-co-IA-co-OEGA) hydrogels, for a constant amount of IA, increases progressively with increasing in OEGA share. On the other hand, the dissociation of carboxyl (-COOH) 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 characterization 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 the P(HEMA-co-IA-co-OEGA) hydrogels can be significantly tuned by variation in their composition. According to all presented, it seems that the obtained copolymeric hydrogels can be a beneficial synergetic combination for controlled delivery of bioactive molecules such as drugs, nucleic acids, peptides, and proteins.

Coaxial electrospun aligned tussah silk fibroin nanostructured fiber scaffolds embedded with hydroxyapatite–tussah silk fibroin nanoparticles for bone tissue engineering

Energy Technology Data Exchange (ETDEWEB)

Shao, Weili [Key Laboratory of Advanced Textile Composites, Ministry of Education, Institute of Textile Composites, Tianjin Polytechnic University, Tianjin 300387 (China); He, Jianxin, E-mail: hejianxin771117@163.com [College of Textiles, Zhongyuan University of Technology, Zhengzhou 450007 (China); Collaborative Innovation Center of Textile and Garment Industry, Henan Province, Zhengzhou 450007 (China); Sang, Feng [Department of Acquired Immune Deficiency Syndrome Treatment and Research Center, The First Affiliated Hospital of Henan University of Traditional Chinese Medicine, Zhengzhou 450007 (China); Ding, Bin [College of Textiles, Zhongyuan University of Technology, Zhengzhou 450007 (China); Collaborative Innovation Center of Textile and Garment Industry, Henan Province, Zhengzhou 450007 (China); Chen, Li, E-mail: chenli@tjpu.edu.cn [Key Laboratory of Advanced Textile Composites, Ministry of Education, Institute of Textile Composites, Tianjin Polytechnic University, Tianjin 300387 (China); Cui, Shizhong; Li, Kejing; Han, Qiming; Tan, Weilin [College of Textiles, Zhongyuan University of Technology, Zhengzhou 450007 (China); Collaborative Innovation Center of Textile and Garment Industry, Henan Province, Zhengzhou 450007 (China)

2016-01-01

The bone is a composite of inorganic and organic materials and possesses a complex hierarchical architecture consisting of mineralized fibrils formed by collagen molecules and coated with oriented hydroxyapatite. To regenerate bone tissue, it is necessary to provide a scaffold that mimics the architecture of the extracellular matrix in native bone. Here, we describe one such scaffold, a nanostructured composite with a core made of a composite of hydroxyapatite and tussah silk fibroin. The core is encased in a shell of tussah silk fibroin. The composite fibers were fabricated by coaxial electrospinning using green water solvent and were characterized using different techniques. In comparison to nanofibers of pure tussah silk, composite notably improved mechanical properties, with 90-fold and 2-fold higher initial modulus and breaking stress, respectively, obtained. Osteoblast-like MG-63 cells were cultivated on the composite to assess its suitability as a scaffold for bone tissue engineering. We found that the fiber scaffold supported cell adhesion and proliferation and functionally promoted alkaline phosphatase and mineral deposition relevant for biomineralization. In addition, the composite were more biocompatible than pure tussah silk fibroin or cover slip. Thus, the nanostructured composite has excellent biomimetic and mechanical properties and is a potential biocompatible scaffold for bone tissue engineering. - Highlights: • A designing scaffold strategy to imitate the mineralized collagen bundles in natural bone was presented. • Aligned nanostructured composite fibers were fabricated by coaxial electrospinning using green water solvent. • Mechanical properties of aligned TSF nanofiber had been significantly improved by embedding with composite nanoparticles. • Composite scaffolds effectively supported proliferation of MG-63 cells and promoted biomineralization.

Biomechanics of Spider Silks

Science.gov (United States)

2006-03-02

water and deformation conditions. Such fibres [Nexia ’ biosteel ’ silk ] were spun from recombinant silk ’cloned’ from Spidroin II and indeed show 67...SUBTITLE 5. FUNDING NUMBERS Biomechanics of Spider Silks F49620-03-1-0111 6. AUTHOR(S) Fritz Vollrath 7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES...Perform Pro, WHSIDIOR, Oct 94 COVER SHEET FINAL (3rd Year) Report to AFOSR on: BIOMECHANICS OF SPIDER SILKS Fritz Vollrath, Oxford University, England

A review on polymeric hydrogel membranes for wound dressing applications: PVA-based hydrogel dressings

Directory of Open Access Journals (Sweden)

Elbadawy A. Kamoun

2017-05-01

Full Text Available This review presents the past and current efforts with a brief description on the featured properties of hydrogel membranes fabricated from biopolymers and synthetic ones for wound dressing applications. Many endeavors have been exerted during past ten years for developing new artificial polymeric membranes, which fulfill the demanded conditions for the treatment of skin wounds. This review mainly focuses on representing specifications of ideal polymeric wound dressing membranes, such as crosslinked hydrogels compatible with wound dressing purposes. But as the hydrogels with single component have low mechanical strength, recent trends have offered composite or hybrid hydrogel membranes to achieve the typical wound dressing requirements.

Hybrid Biodegradable Hydrogels Obtained from Nanoclay and Carboxymethylcellulose Polysaccharide: Hydrophilic, Kinetic, Spectroscopic and Morphological Properties.

Science.gov (United States)

Nascimento, Denis W S; de Moura, Márcia R; Mattoso, Luiz H C; Aouada, Fauze A

2017-01-01

In this paper, series of novel nanocomposite hydrogels based on polyacrylamide (PAAm), carboxymethylcellulose (CMC) and nanoclay were synthesized. Hydrophilic, kinetic, spectroscopic and morphological properties were investigated as function of their constituents. Spectroscopic properties confirmed the obtaining of the nanocomposites. It was also observed that the nanocomposites have walls of pores with a more rugged morphology compared with the morphology of the hydrogel without clay, contributing to repel the water molecules. Besides, the results showed that the velocity and quantity of water uptake may be controlled by adjusting of matrix rigidity, i.e., nanoclay content into polymeric matrix. This behavior is required to future application in agriculture fields, specifically as carrier vehicle in controlled release of agrochemicals. Thus, these nanocomposites have technological application.

Characterization and mechanical performance study of silk/PVA cryogels: towards nucleus pulposus tissue engineering.

Science.gov (United States)

Neo, Puay Yong; Shi, Pujiang; Goh, James Cho-Hong; Toh, Siew Lok

2014-10-20

Poly (vinyl) alcohol (PVA) cryogels are reported in the literature for application in nucleus pulposus (NP) replacement strategies. However, these studies are mainly limited to acellular approaches-in part due to the high hydrophilicity of PVA gels that renders cellular adhesion difficult. Silk is a versatile biomaterial with excellent biocompatibility. We hypothesize that the incorporation of silk with PVA will (i) improve the cell-hosting abilities of PVA cryogels and (ii) allow better tailoring of physical properties of the composite cryogels for an NP tissue engineering purpose. 5% (wt/vol) PVA is blended with 5% silk fibroin (wt/vol) to investigate the effect of silk : PVA ratios on the cryogels' physical properties. Results show that the addition of silk results in composite cryogels that are able to swell to more than 10 times its original dry weight and rehydrate to at least 70% of its original wet weight. Adding at least 20% silk significantly improves surface hydrophobicity and is correlated with an improvement in cell-hosting abilities. Cell-seeded cryogels also display an increment in compressive modulus and hoop stress values. In all, adding silk to PVA creates cryogels that can be potentially used as NP replacements.

Recombinant spider silk genetically functionalized with affinity domains.

Science.gov (United States)

Jansson, Ronnie; Thatikonda, Naresh; Lindberg, Diana; Rising, Anna; Johansson, Jan; Nygren, Per-Åke; Hedhammar, My

2014-05-12

Functionalization of biocompatible materials for presentation of active protein domains is an area of growing interest. Herein, we describe a strategy for functionalization of recombinant spider silk via gene fusion to affinity domains of broad biotechnological use. Four affinity domains of different origin and structure; the IgG-binding domains Z and C2, the albumin-binding domain ABD, and the biotin-binding domain M4, were all successfully produced as soluble silk fusion proteins under nondenaturing purification conditions. Silk films and fibers produced from the fusion proteins were demonstrated to be chemically and thermally stable. Still, the bioactive domains are concluded to be folded and accessible, since their respective targets could be selectively captured from complex samples, including rabbit serum and human plasma. Interestingly, materials produced from mixtures of two different silk fusion proteins displayed combined binding properties, suggesting that tailor-made materials with desired stoichiometry and surface distributions of several binding domains can be produced. Further, use of the IgG binding ability as a general mean for presentation of desired biomolecules could be demonstrated for a human vascular endothelial growth factor (hVEGF) model system, via a first capture of anti-VEGF IgG to silk containing the Z-domain, followed by incubation with hVEGF. Taken together, this study demonstrates the potential of recombinant silk, genetically functionalized with affinity domains, for construction of biomaterials capable of presentation of almost any desired biomolecule.

Development of hydrogels composites for potential use as biomaterials

International Nuclear Information System (INIS)

Silva, Gabriela T. da; Alves, Natali O.; Schulz, Gracelie A.S.; Fajardo, Andre R.

2015-01-01

Hydrogels, three-dimensional polymer networks that can absorb and retain impressive amounts of liquid, have shown a remarkable evolution in the past years. Since their first description, the hydrogels have replaced their inert characteristic by smart properties, which help enlarging the range of applicability of such soft materials in different fields. Hydrogels had been prepared from various polymers (including synthetic or natural or both), which allows obtaining materials with unique and desirable properties. This work deals with the preparation of hydrogels and hydrogel composites based on a synthetic/natural hybrid polymer network filled with bovine bone powder, which is composed mainly by hydroxyapatite (as inorganic phase) and collagen (as organic phase). The resulting materials were characterized by DRX, FTIR and TGA analyses. Additionally, water uptake capacity was estimated for both hydrogels and hydrogels composites samples by swelling assays. (author)

Tunable Collagen I Hydrogels for Engineered Physiological Tissue Micro-Environments

Science.gov (United States)

Antoine, Elizabeth E.; Vlachos, Pavlos P.; Rylander, Marissa N.

2015-01-01

Collagen I hydrogels are commonly used to mimic the extracellular matrix (ECM) for tissue engineering applications. However, the ability to design collagen I hydrogels similar to the properties of physiological tissues has been elusive. This is primarily due to the lack of quantitative correlations between multiple fabrication parameters and resulting material properties. This study aims to enable informed design and fabrication of collagen hydrogels in order to reliably and reproducibly mimic a variety of soft tissues. We developed empirical predictive models relating fabrication parameters with material and transport properties. These models were obtained through extensive experimental characterization of these properties, which include compression modulus, pore and fiber diameter, and diffusivity. Fabrication parameters were varied within biologically relevant ranges and included collagen concentration, polymerization pH, and polymerization temperature. The data obtained from this study elucidates previously unknown fabrication-property relationships, while the resulting equations facilitate informed a priori design of collagen hydrogels with prescribed properties. By enabling hydrogel fabrication by design, this study has the potential to greatly enhance the utility and relevance of collagen hydrogels in order to develop physiological tissue microenvironments for a wide range of tissue engineering applications. PMID:25822731

Enhancing analysis of cells and proteins by fluorescence imaging on silk-based biomaterials: modulating the autofluorescence of silk.

Science.gov (United States)

Neo, Puay Yong; Tan, Daryl Jian-An; Shi, Pujiang; Toh, Siew Lok; Goh, James Cho-Hong

2015-02-01

Silk is a versatile and established biomaterial for various tissue engineering purposes. However, it also exhibits strong autofluorescence signals-thereby hindering fluorescence imaging analysis of cells and proteins on silk-derived biomaterials. Sudan Black B (SB) is a lysochrome dye commonly used to stain lipids in histology. It has also been reported to be able to quench autofluorescence of tissues in histology and has been tested on artificial biomedical polymers in recent years. It was hypothesized that SB would exert similar quenching effects on silk, modulating the autofluorescence signals, and thereby enabling improved imaging analysis of cells and molecules of interests. The quenching effect of SB on the intrinsic fluorescence properties of silk and on commercial fluorescent dyes were first investigated in this study. SB was then incorporated into typical fluorescence-based staining protocols to study its effectiveness in improving fluorescence-based imaging of the cells and proteins residing with the silk-based biomaterials. Silk processed into various forms of biomaterials (e.g., films, sponges, fibers, and electrospun mats) was seeded with cells and cultured in vitro. At sacrificial time points, specimens were harvested, fixed, and prepared for fluorescence staining. SB, available commercially as a powder, was dissolved in 70% ethanol (0.3% [w/v]) to form staining solutions. SB treatment was introduced at the last step of typical immunofluorescence staining protocols for 15-120 min. For actin staining protocols by phalloidin toxin, SB staining solutions were added before and after permeabilization with Triton-X for 15-30 min. Results showed that ideal SB treatment duration is about 15 min. Apart from being able to suppress the autofluorescence of silk, this treatment duration was also not too long to adversely affect the fluorescent labeling probes used. The relative improvement brought about by SB treatment was most evident in the blue and green

Photocrosslinked nanocomposite hydrogels from PEG and silica nanospheres: Structural, mechanical and cell adhesion characteristics

International Nuclear Information System (INIS)

Gaharwar, Akhilesh K.; Rivera, Christian; Wu, Chia-Jung; Chan, Burke K.; Schmidt, Gudrun

2013-01-01

Photopolymerized hydrogels are extensively investigated for various tissue engineering applications, primarily due to their ability to form hydrogels in a minimally invasive manner. Although photocrosslinkable hydrogels provide necessary biological and chemical characteristics to mimic cellular microenvironments, they often lack sufficient mechanical properties. Recently, nanocomposite approaches have demonstrated potential to overcome these deficits by reinforcing the hydrogel network with. In this study, we investigate some physical, chemical, and biological properties of photocrosslinked poly(ethylene glycol) (PEG)-silica hydrogels. The addition of silica nanospheres significantly suppresses the hydration degree of the PEG hydrogels, indicating surface interactions between the silica nanospheres and the polymer chains. No significant change in hydrogel microstructure or average pore size due to the addition of silica nanospheres was observed. However, addition of silica nanospheres significantly increases both the mechanical strength and the toughness of the hydrogel networks. The biological properties of these nanocomposite hydrogels were evaluated by seeding fibroblast cells on the hydrogel surface. While the PEG hydrogels showed minimum cell adhesion, spreading and proliferation, the addition of silica nanospheres enhanced initial cell adhesion, promoted cell spreading and increased the metabolic activity of the cells. Overall, results indicate that the addition of silica nanospheres improves the mechanical stiffness and cell adhesion properties of PEG hydrogels and can be used for biomedical applications that required controlled cell adhesion. - Graphical abstract: Structural, mechanical and biological properties of photocrosslinked nanocomposite hydrogels from silica and poly(ethylene oxide) are investigated. Silica reinforce the hydrogel network and improved mechanical strength. Addition of induces cell adhesion characteristic properties for various

Effect of Acid Hydrolysis and Thermal Hydrolysis on Solubility and Properties of Oil Palm Empty Fruit Bunch Fiber Cellulose Hydrogel

Directory of Open Access Journals (Sweden)

Sinyee Gan

2015-11-01

Full Text Available Cellulose hydrogel was produced from pretreated oil palm empty fruit bunch fiber (EFB that went through acid hydrolysis and thermal hydrolysis. The pretreated EFB was dissolved in LiOH/urea aqueous solution using the rapid dissolution method and was subjected to a crosslinking process with the aid of epichlorohydrin to form hydrogel. The effects of both hydrolyses’ time on average molecular weight (Mŋ, solubility, and properties of EFB hydrogels were evaluated. Both hydrolyses led to lower Mŋ, lower crystallinity index (CrI and hence, resulted in higher cellulose solubility. X-ray diffraction (XRD characterization revealed the CrI and transition of crystalline structure of EFB from cellulose I to II. The effects of hydrolysis time on the transparency, degree of swelling (DS, and morphology of the regenerated cellulose hydrogel were also investigated using an ultraviolet-visible (UV-Vis spectrophotometer and a Field emission scanning electron microscope (FESEM, respectively. These findings provide an efficient method to improve the solubility and properties of regenerated cellulose products.

Exploring the Properties of Genetically Engineered Silk-Elastin-Like Protein Films.

Science.gov (United States)

Machado, Raul; da Costa, André; Sencadas, Vitor; Pereira, Ana Margarida; Collins, Tony; Rodríguez-Cabello, José Carlos; Lanceros-Méndez, Senentxu; Casal, Margarida

2015-12-01

Free standing films of a genetically engineered silk-elastin-like protein (SELP) were prepared using water and formic acid as solvents. Exposure to methanol-saturated air promoted the formation of aggregated β-strands rendering aqueous insolubility and improved the mechanical properties leading to a 10-fold increase in strain-to-failure. The films were optically clear with resistivity values similar to natural rubber and thermally stable up to 180 °C. Addition of glycerol showed to enhance the flexibility of SELP/glycerol films by interacting with SELP molecules through hydrogen bonding, interpenetrating between the polymer chains and granting more conformational freedom. This detailed characterization provides cues for future and unique applications using SELP based biopolymers. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene oxide from silk cocoon: a novel magnetic fluorophore for multi-photon imaging

OpenAIRE

Roy, Manas; Kusurkar, Tejas Sanjeev; Maurya, Sandeep Kumar; Meena, Sunil Kumar; Singh, Sushil Kumar; Sethy, Niroj; Bhargava, Kalpana; Sharma, Raj Kishore; Goswami, Debabrata; Sarkar, Sabyasachi; Das, Mainak

2013-01-01

In this work, we synthesized graphene oxide from silk cocoon embarking its new dimension as a magnetic fluorophore when compared with its present technical status, which at best is for extracting silk as a biomaterial for tissue engineering applications. We produced graphene oxide by pyrolysing the silk cocoon in an inert atmosphere. The collected raw carbon is oxidized by nitric acid that readily produces multilayer graphene oxide with nano carbon particulates. Structural properties of the g...

Silk fibroin as biomaterial for bone tissue engineering.

Science.gov (United States)

Melke, Johanna; Midha, Swati; Ghosh, Sourabh; Ito, Keita; Hofmann, Sandra

2016-02-01

Silk fibroin (SF) is a fibrous protein which is produced mainly by silkworms and spiders. Its unique mechanical properties, tunable biodegradation rate and the ability to support the differentiation of mesenchymal stem cells along the osteogenic lineage, have made SF a favorable scaffold material for bone tissue engineering. SF can be processed into various scaffold forms, combined synergistically with other biomaterials to form composites and chemically modified, which provides an impressive toolbox and allows SF scaffolds to be tailored to specific applications. This review discusses and summarizes recent advancements in processing SF, focusing on different fabrication and functionalization methods and their application to grow bone tissue in vitro and in vivo. Potential areas for future research, current challenges, uncertainties and gaps in knowledge are highlighted. Silk fibroin is a natural biomaterial with remarkable biomedical and mechanical properties which make it favorable for a broad range of bone tissue engineering applications. It can be processed into different scaffold forms, combined synergistically with other biomaterials to form composites and chemically modified which provides a unique toolbox and allows silk fibroin scaffolds to be tailored to specific applications. This review discusses and summarizes recent advancements in processing silk fibroin, focusing on different fabrication and functionalization methods and their application to grow bone tissue in vitro and in vivo. Potential areas for future research, current challenges, uncertainties and gaps in knowledge are highlighted. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Silk Fibroin Aqueous-Based Adhesives Inspired by Mussel Adhesive Proteins.

Science.gov (United States)

Burke, Kelly A; Roberts, Dane C; Kaplan, David L

2016-01-11

Silk fibroin from the domesticated silkworm Bombyx mori is a naturally occurring biopolymer with charged hydrophilic terminal regions that end-cap a hydrophobic core consisting of repeating sequences of glycine, alanine, and serine residues. Taking inspiration from mussels that produce proteins rich in L-3,4-dihydroxyphenylalanine (DOPA) to adhere to a variety of organic and inorganic surfaces, the silk fibroin was functionalized with catechol groups. Silk fibroin was selected for its high molecular weight, tunable mechanical and degradation properties, aqueous processability, and wide availability. The synthesis of catechol-functionalized silk fibroin polymers containing varying amounts of hydrophilic polyethylene glycol (PEG, 5000 g/mol) side chains was carried out to balance silk hydrophobicity with PEG hydrophilicity. The efficiency of the catechol functionalization reaction did not vary with PEG conjugation over the range studied, although tuning the amount of PEG conjugated was essential for aqueous solubility. Adhesive bonding and cell compatibility of the resulting materials were investigated, where it was found that incorporating as little as 6 wt % PEG prior to catechol functionalization resulted in complete aqueous solubility of the catechol conjugates and increased adhesive strength compared with silk lacking catechol functionalization. Furthermore, PEG-silk fibroin conjugates maintained their ability to form β-sheet secondary structures, which can be exploited to reduce swelling. Human mesenchymal stem cells (hMSCs) proliferated on the silks, regardless of PEG and catechol conjugation. These materials represent a protein-based approach to catechol-based adhesives, which we envision may find applicability as biodegradable adhesives and sealants.

Nanostructure and molecular mechanics of spider dragline silk protein assemblies

Science.gov (United States)

Keten, Sinan; Buehler, Markus J.

2010-01-01

Spider silk is a self-assembling biopolymer that outperforms most known materials in terms of its mechanical performance, despite its underlying weak chemical bonding based on H-bonds. While experimental studies have shown that the molecular structure of silk proteins has a direct influence on the stiffness, toughness and failure strength of silk, no molecular-level analysis of the nanostructure and associated mechanical properties of silk assemblies have been reported. Here, we report atomic-level structures of MaSp1 and MaSp2 proteins from the Nephila clavipes spider dragline silk sequence, obtained using replica exchange molecular dynamics, and subject these structures to mechanical loading for a detailed nanomechanical analysis. The structural analysis reveals that poly-alanine regions in silk predominantly form distinct and orderly beta-sheet crystal domains, while disorderly regions are formed by glycine-rich repeats that consist of 31-helix type structures and beta-turns. Our structural predictions are validated against experimental data based on dihedral angle pair calculations presented in Ramachandran plots, alpha-carbon atomic distances, as well as secondary structure content. Mechanical shearing simulations on selected structures illustrate that the nanoscale behaviour of silk protein assemblies is controlled by the distinctly different secondary structure content and hydrogen bonding in the crystalline and semi-amorphous regions. Both structural and mechanical characterization results show excellent agreement with available experimental evidence. Our findings set the stage for extensive atomistic investigations of silk, which may contribute towards an improved understanding of the source of the strength and toughness of this biological superfibre. PMID:20519206

Feeding Single-Walled Carbon Nanotubes or Graphene to Silkworms for Reinforced Silk Fibers.

Science.gov (United States)

Wang, Qi; Wang, Chunya; Zhang, Mingchao; Jian, Muqiang; Zhang, Yingying

2016-10-12

Silkworm silk is gaining significant attention from both the textile industry and research society because of its outstanding mechanical properties and lustrous appearance. The possibility of creating tougher silks attracts particular research interest. Carbon nanotubes and graphene are widely studied for their use as reinforcement. In this work, we report mechanically enhanced silk directly collected by feeding Bombyx mori larval silkworms with single-walled carbon nanotubes (SWNTs) and graphene. We found that parts of the fed carbon nanomaterials were incorporated into the as-spun silk fibers, whereas the others went into the excrement of silkworms. Spectroscopy study indicated that nanocarbon additions hindered the conformation transition of silk fibroin from random coil and α-helix to β-sheet, which may contribute to increased elongation at break and toughness modules. We further investigated the pyrolysis of modified silk, and a highly developed graphitic structure with obviously enhanced electrical conductivity was obtained through the introduction of SWNTs and graphene. The successful generation of these SWNT- or graphene-embedded silks by in vivo feeding is expected to open up possibilities for the large-scale production of high-strength silk fibers.

Dextran/Albumin hydrogel sealant for Dacron(R) vascular prosthesis.

Science.gov (United States)

Lisman, Anna; Butruk, Beata; Wasiak, Iga; Ciach, Tomasz

2014-05-01

In this paper, the authors describe a novel type of hydrogel coating prepared from the copolymer of human serum albumin and oxidized dextran. The material was designed as a hydrogel sealant for polyester (Dacron®)-based vascular grafts. Dextran was chosen as a coating material due to its anti-thrombogenic properties. Prepared hydrogels were compared with similar, already known biomaterial made from gelatine with the same cross-linking agent. Obtained hydrogels, prepared from various ratios of oxidized dextran/albumin or oxidized dextran/gelatine, showed different cross-linking densities, which caused differences in swelling, degradation rate and mechanical properties. Permeability tests confirmed the complete tightness of the hydrogel-modified prosthesis. Results showed that application of the hydrogel coating provided leakage-free prosthesis and eliminated the need of pre-clotting.

Photo-cross-linked PLA-PEO-PLA hydrogels from self-assembled physical networks: mechanical properties and influence of assumed constitutive relationships.

Science.gov (United States)

Sanabria-DeLong, Naomi; Crosby, Alfred J; Tew, Gregory N

2008-10-01

Poly(lactide)-block-poly(ethylene oxide)-block-poly(lactide) (PLA-PEO-PLA) triblock copolymers are known to form physical hydrogels in water as a result of the polymer's amphiphilicity. Their mechanical properties, biocompatibility, and biodegradability have made them attractive for use as soft tissue scaffolds. However, the network junction points are not covalently cross-linked, and in a highly aqueous environment these hydrogels adsorb more water, transform from gel to sol, and lose the designed mechanical properties. In this article, a hydrogel was formed by the use of a novel two-step approach. In the first step, the end-functionalized PLA-PEO-PLA triblock was self-assembled into a physical hydrogel through hydrophobic micelle network junctions, and in the second step, this self-assembled physical network structure was locked into place by photo-cross-linking the terminal acrylate groups. In contrast with physical hydrogels, the photo-cross-linked gels remained intact in phosphate-buffered solution at body temperature. The swelling, degradation, and mechanical properties were characterized, and they demonstrated an extended degradation time (approximately 65 days), an exponential decrease in modulus with degradation time, and a tunable shear modulus (1.6-133 kPa). We also discuss the various constitutive relationships (Hookean, neo-Hookean, and Mooney-Rivlin) that can be used to describe the stress-strain behavior of these hydrogels. The chosen model and assumptions used for data fitting influenced the obtained modulus values by as much as a factor of 3.5, which demonstrates the importance of clearly stating one's data fitting parameters so that accurate comparisons can be made within the literature.

Development of a novel sodium fusidate-loaded triple polymer hydrogel wound dressing: Mechanical properties and effects on wound repair.

Science.gov (United States)

Jin, Sung Giu; Kim, Kyeong Soo; Kim, Dong Wuk; Kim, Dong Shik; Seo, Youn Gee; Go, Toe Gyung; Youn, Yu Seok; Kim, Jong Oh; Yong, Chul Soon; Choi, Han-Gon

2016-01-30

To develop a novel sodium fusidate-loaded triple polymer hydrogel dressing (TPHD), numerious polyvinyl alcohol-based (PVA) hydrogel dressings were prepared with various hydrophilic polymers using the freeze-thaw method, and their hydrogel dressing properties were assessed. Among the hydrophilic polymers tested, sodium alginate (SA) improved the swelling capacity the most, and polyvinyl pyrrolidone (PVP) provided the greatest improvement in bioadhesive stength and mechanical properties. Thus, PVA based-TPHDs were prepared using different ratios of PVP:SA. The effect of selected PVP:SA ratios on the swelling capacity, bioadhesive strength, mechanical properties, and drug release, permeation and deposition characteristics of sodium fusidate-loaded PVA-based TPHDs were assessed. As the ratio of PVP:SA increased in PVA-loaded TPHD, the swelling capacity, mechanical properties, drug release, permeation and deposition were improved. The TPHD containing PVA, PVP, SA and sodium fusidate at the weight ratio of 10/6/1/1 showed excellent hydrogel dressing properties, release, permeation and deposition of drug. Within 24h, 71.8 ± 1.3% of drug was released. It permeated 625.1 ± 81.2 μg/cm(2) through the skin and deposited of 313.8 ± 24.1 μg/cm(2) within 24h. The results of in vivo pharmacodynamic studies showed that sodium fusidate-loaded TPHD was more effective in improving the repair process than was a commercial product. Thus, this sodium fusidate-loaded TPHD could be a novel tool in wound care. Copyright © 2015 Elsevier B.V. All rights reserved.

Synthesis and characterization of dense membranes of silk fibroin with glycerin

International Nuclear Information System (INIS)

Silva, Mariana F.; Moraes, Mariana A. de; Weska, Raquel F.; Nogueira, Grinia M.; Beppu, Marisa M.

2009-01-01

The addition of plasticizers seeks improvements in mechanical properties of dense membranes of silk fibroin with possible interactions by hydrogen bonds. The aim of the present study was to produce and characterize dense membranes of silk fibroin containing glycerin in two different concentrations. The characterization of the membranes was performed from scanning electron microscopy (SEM), mechanical traction tests, infrared spectroscopy (FTIR-ATR) and X-ray diffraction (XRD). The results indicated that the addition of glycerin allowed obtaining homogeneous and more crystalline membranes and improved their properties of elongation. (author)

A study on radiation-induced graft copolymerization of monomer onto natural silk fabric

International Nuclear Information System (INIS)

Xiang Zhengyu; Wan Dairong; He Qian

1995-02-01

In order to improve the properties of natural silk fabric, the mechanism and method of the radiation induced graft copolymerization of monomers onto natural silk fabric were studied. Three monomers, acrylamide, methylacrylamide and hydroxymethyl acrylamide, were selected for grafting test according to requirements of graft processing. The processing conditions of monomer infusion were studied. The properties of grafted samples were measured. The results are as follows: the rate of weight increasing is 10%∼29%; the rate of thickness increasing is 5%∼20%; the abrupt elasticity rose by 30%; the retarded elasticity rose by 12%; wet elasticity rose by 40%; and the brightness of colour and lustre were improved. It is concluded that while the radiation grafted silk kept its natural characteristics, other properties were improved. It became even chubby and thicker. (4 refs., 3 figs., 3 tabs.)

Untangling spider silk evolution with spidroin terminal domains

Directory of Open Access Journals (Sweden)

Garb Jessica E

2010-08-01

assembly. Phylogenetic analyses of the conserved N- and C-terminal domains illustrate dramatic radiation of the spidroin gene family, involving extensive duplications, shifts in expression patterns and extreme diversification of repetitive structural sequences that endow spider silks with an unparalleled range of mechanical properties.

Influence of dissolution processing of PVA blends on the characteristics of their hydrogels synthesized by radiation—Part I: Gel fraction, swelling, and mechanical properties

International Nuclear Information System (INIS)

Alcântara, M.T.S.; Brant, A.J.C.; Giannini, D.R.; Pessoa, J.O.C.P.; Andrade, A.B.; Riella, H.G.; Lugão, A.B.

2012-01-01

In this work several hydrogels were obtained with two different poly(vinyl alcohol)s/PVAs as the main polymer in aqueous solutions containing 10% of PVA, 0.6% of agar, and 0.6% of κ-carrageenan (KC), cross-linked by gamma-rays from a 60 Co irradiation source. The PVAs tested have different degrees of hydrolysis and viscosities at 4% with values closed to 30 mPa s. The aqueous polymeric solutions were prepared using two distinct processes: the simple process of heating–stirring and that of making use of an autoclave. The purpose of this study was to evaluate the influence of the dissolution process by means of both methods on the hydrogels’ properties obtained. These were investigated by means of degree of cross-linking/gel fraction, degree of swelling in water, and some mechanical properties. The results that are obtained for hydrogels synthesized from solutions of PVA, agar, KC, and blends thereof prepared by both dissolution processes showed higher degrees of swelling for hydrogels from the autoclaved polymer solutions than those from the solutions prepared by simple heating–stirring process. Furthermore, their hydrogels containing totally hydrolyzed PVA displayed higher tensile strength and lower elongation properties. - Highlights: ► Hydrogels from γ-irradiated PVA and PVA-polysaccharide blends were obtained. ► PVA molar mass and degree of hydrolysis play an important role in their hydrogels. ► Dissolution processes of PVAs have influenced on their hydrogel characteristics. ► Degrees of swelling of hydrogels were lower when prepared from autoclaved solutions.

Supramolecular polyaniline hydrogel as a support for urease

International Nuclear Information System (INIS)

Słoniewska, Anna; Pałys, Barbara

2014-01-01

Supramolecular hydrogels of conducting polymers are successfully used in bioelectrochemistry because of their mechanical and swelling properties of gels added to the specific electron transport properties of conducting polymers. We have studied polyaniline-poly(styrene sulfonate) (PANI–PSS) hydrogel as a substrate for the urease. The hydrogels were synthesized at pH = 0 and pH = 5. PANI–PSS hydrogel is a supramolecular self-assembly material consisting of positively-charged PANI chains and negatively-charged PSS chains. The hydrogel was studied by cyclic voltammetry, infrared and Raman spectroscopy and Scanning Electron Microscopy (SEM). Raman spectra revealed presence of phenazine rings in the hydrogel structure. Phenazine rings form covalent cross-linkers contributing to the hydrogel mechanical stability. The covalent cross-linkers influence the cyclic voltammetry responses of the hydrogel in acidic media. We tested the activity of urease immobilized in the PANI–PSS hydrogel by the physical adsorption or by the covalent bonding with the carbodiimide reaction. The enzyme immobilized in hydrogels prepared at higher pH value reveals significantly higher sensitivity. The method of the enzyme immobilization has smaller impact on the sensitivity. All hydrogel sensors reveal largely higher sensitivity to urea comparing to urease immobilized in the typical electrochemically deposited PANI films. The sensitivity of urease covalently bond to the hydrogel obtained at pH = 5 was as high as 1693 μA/(mol dm 3 ). The sensor response was linear in the urea concentration range from 10 −4 to 7 × 10 −2 mol/dm 3

Natural Occurring Silks and Their Analogues as Materials for Nerve Conduits

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Christine Radtke

2016-10-01

Full Text Available Spider silk and its synthetic derivatives have a light weight in combination with good strength and elasticity. Their high cytocompatibility and low immunogenicity make them well suited for biomaterial products such as nerve conduits. Silk proteins slowly degrade enzymatically in vivo, thus allowing for an initial therapeutic effect such as in nerve scaffolding to facilitate endogenous repair processes, and then are removed. Silks are biopolymers naturally produced by many species of arthropods including spiders, caterpillars and mites. The silk fibers are secreted by the labial gland of the larvae of some orders of Holometabola (insects with pupa or the spinnerets of spiders. The majority of studies using silks for biomedical applications use materials from silkworms or spiders, mostly of the genus Nephila clavipes. Silk is one of the most promising biomaterials with effects not only in nerve regeneration, but in a number of regenerative applications. The development of silks for human biomedical applications is of high scientific and clinical interest. Biomaterials in use for biomedical applications have to meet a number of requirements such as biocompatibility and elicitation of no more than a minor inflammatory response, biodegradability in a reasonable time and specific structural properties. Here we present the current status in the field of silk-based conduit development for nerve repair and discuss current advances with regard to potential clinical transfer of an implantable nerve conduit for enhancement of nerve regeneration.

Extracted sericin from silk waste for film formation

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Rungsinee Sothornvit

2010-03-01

Full Text Available Sericin is the second main component in cocoons, which are removed in the silk reeling process of the raw silk industry and in the silk waste degumming of the spun silk industry. The main amino acid of sericin, serine, exhibits a skin moisturing and antiwrinkle action, which is interesting to use for film formation in this study. The extraction conditions of sericin from two silk wastes, pieced cocoon and inferior knubbs were studied to find the optimum extraction conditions. Boiling water extraction was considered based on the response surface methodology (RSM in order to identify the important factors for the sericin extraction. The two factors considered were time and temperature. Both factors were needed to be independent parameters in the predicted equation in order to improve the model fit with R2 = 0.84. The components ofextracted sericin were 18.24% serine, 9.83% aspatate, and 5.51% glycine with a molecular weight of 132 kDa. Film formationfrom extracted sericin was carried out to find the optimum conditions. Extracted sericin could not form a stand-alonefilm. Therefore, polysaccharide polymers, such as glucomannan, were incorporated with glycerol to form a flexible film.Sericin-based films were characterized for its properties in terms of solubility and permeability before application. It wasfound that sericin-based films showed a film flexibility and solubility without an increasing film water vapor permeability.

Formation of zeolite A. Properties of the alumina--silicate hydrogel. Formation of zeolite A on prolonged maturation of the hydrogel

Energy Technology Data Exchange (ETDEWEB)

Polak, F; Cichocki, A

1974-01-01

Analytic, adsorption, and x-ray investigations of a maturated hydrogel A, crystallized at 94/sup 0/ during 6 hr and of a hydrogel A kept for 2 months at room temperature showed that the zeolite A was formed easily and that maturation of the hydrogel A had little effect on its crystallization at 94/sup 0/. The hydrogel A kept for 2 months at room temperature passed almost completely into the crystalline zeolite A. Changes in the content of SiO/sub 2/, Al/sub 2/O/sub 3/, and Na/sub 2/O in the liquid and solid phases during the maturation and crystallization of the hydrogels A were studied.

Silk fibers and silk-producing organs of Harpactea rubicunda (C. L. Koch 1838) (Araneae, Dysderidae).

Science.gov (United States)

Hajer, Jaromír; Malý, Jan; Reháková, Dana

2013-01-01

Scanning electron microscopy and atomic force microscopy were used to study the silk spinning apparatus and silks of Harpactea rubicunda spiders. Three types of silk secretions that are produced by three kinds of silk spinning glands (ampullate, piriform, and pseudaciniform) and released through three types of spigots, were confirmed for both adult and juvenile spiders. Silk secretions for the construction of spider webs for shelter or retreat are produced by the pseudaciniform silk glands. Silk secretions that are released from spigots in the course of web construction are not processed by the legs during the subsequent process of hardening. Pairs of nanofibril bundles seemed to be part of the basic microarchitecture of the web silk fibers as revealed by AFM. These fiber bundles frequently not only overlap one another, but occasionally also interweave. This structural variability may strengthen the spider web. High-resolution AFM scans of individual nanofibrils show a distinctly segmented nanostructure. Each globular segment is ∼30-40 nm long along the longitudinal axis of the fiber, and resembles a nanosegment of artificial fibroin described by Perez-Rigueiro et al. (2007). Copyright © 2012 Wiley Periodicals, Inc.

Charged Triazole Cross-Linkers for Hyaluronan-Based Hybrid Hydrogels

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Maike Martini

2016-09-01

Full Text Available Polyelectrolyte hydrogels play an important role in tissue engineering and can be produced from natural polymers, such as the glycosaminoglycan hyaluronan. In order to control charge density and mechanical properties of hyaluronan-based hydrogels, we developed cross-linkers with a neutral or positively charged triazole core with different lengths of spacer arms and two terminal maleimide groups. These cross-linkers react with thiolated hyaluronan in a fast, stoichiometric thio-Michael addition. Introducing a positive charge on the core of the cross-linker enabled us to compare hydrogels with the same interconnectivity, but a different charge density. Positively charged cross-linkers form stiffer hydrogels relatively independent of the size of the cross-linker, whereas neutral cross-linkers only form stable hydrogels at small spacer lengths. These novel cross-linkers provide a platform to tune the hydrogel network charge and thus the mechanical properties of the network. In addition, they might offer a wide range of applications especially in bioprinting for precise design of hydrogels.

Synthetic Biodegradable Hydrogels with Excellent Mechanical Properties and Good Cell Adhesion Characteristics Obtained by the Combinatorial Synthesis of Photo-Cross-Linked Networks

NARCIS (Netherlands)

Zant, Erwin; Grijpma, Dirk W.

Major drawbacks of synthetic hydrogels are their poor mechanical properties and their limited ability to allow cell attachment and proliferation. By photo-cross-linking mixtures of dimethacrylate-functionalized oligomers (macromers) in a combinatorial manner in solution, synthetic hydrogels with

Anisotropic dehydration of hydrogel surfaces.

Science.gov (United States)

Kaklamani, Georgia; Cheneler, David; Grover, Liam M; Adams, Michael J; Anastasiadis, Spiros H; Bowen, James

2017-12-01

Efforts to develop tissue-engineered skin for regenerative medicine have explored natural, synthetic, and hybrid hydrogels. The creation of a bilayer material, with the stratification exhibited by native skin, is a complex problem. The mechanically robust, waterproof epidermis presents the stratum corneum at the tissue/air interface, which confers many of these protective properties. In this work, we explore the effect of high temperatures on alginate hydrogels, which are widely employed for tissue engineering due to their excellent mechanical properties and cellular compatibility. In particular, we investigate the rapid dehydration of the hydrogel surface which occurs following local exposure to heated surfaces with temperatures in the range 100-200 °C. We report the creation of a mechanically strengthened hydrogel surface, with improved puncture resistance and increased coefficient of friction, compared to an unheated surface. The use of a mechanical restraint during heating promoted differences in the rate of mass loss; the rate of temperature increase within the hydrogel, in the presence and absence of restraint, is simulated and discussed. It is hoped that the results will be of use in the development of processes suitable for preparing skin-like analogues; application areas could include wound healing and skin restoration.

Engineering three-dimensional cell mechanical microenvironment with hydrogels.

Science.gov (United States)

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.

Engineering three-dimensional cell mechanical microenvironment with hydrogels

International Nuclear Information System (INIS)

Huang Guoyou; Wang Lin; Han Yulong; Zhang Qiancheng; Xu Feng; Lu Tianjian; Wang Shuqi; Wu Jinhui

2012-01-01

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. (topical review)

Preparation of highly absorbing polymeric hydrogels by radiation processing: mechanical and physical properties

International Nuclear Information System (INIS)

Dragusin, M.

1994-01-01

Some highly absorbing polymeric hydrogels such as acrylic polymers were produced by radiation processing with gamma sources Co-60 of 10,000 Ci, 3 kGy/h and an electron beam accelerator of 3 - 6 MeV, 0.3 - 3 kGy/s. For practical purposes, such as different applications in agriculture, etc, we studied the physical properties of residual monomers by refractometric and polarographic methods and the mechanical properties (gel strength) with devices made in our laboratory. (Author)

Water-based preparation of spider silk films as drug delivery matrices.

Science.gov (United States)

Agostini, Elisa; Winter, Gerhard; Engert, Julia

2015-09-10

The main focus of this work was to obtain a drug delivery matrix characterized by biocompatibility, water insolubility and good mechanical properties. Moreover the preparation process has to be compatible with protein encapsulation and the obtained matrix should be able to sustain release a model protein. Spider silk proteins represent exceptional natural polymers due to their mechanical properties in combination with biocompatibility. As both hydrophobic and slowly biodegrading biopolymers, recombinant spider silk proteins fulfill the required properties for a drug delivery system. In this work, we present the preparation of eADF4(C16) films as drug delivery matrices without the use of any organic solvent. Water-based spider silk films were characterized in terms of protein secondary structure, thermal stability, zeta-potential, solubility, mechanical properties, and water absorption and desorption. Additionally, this study includes an evaluation of their application as a drug delivery system for both small molecular weight drugs and high molecular weight molecules such as proteins. Our investigation focused on possible improvements in the film's mechanical properties including plasticizers in the film matrix. Furthermore, different film designs were prepared, such as: monolayer, coated monolayer, multilayer (sandwich), and coated multilayer. The release of the model protein BSA from these new systems was studied. Results indicated that spider silk films are a promising protein drug delivery matrix, capable of releasing the model protein over 90 days with a release profile close to zero order kinetic. Such films could be used for several pharmaceutical and medical purposes, especially when mechanical strength of a drug eluting matrix is of high importance. Copyright © 2015 Elsevier B.V. All rights reserved.

Novel silk fibroin films prepared by formic acid/hydroxyapatite dissolution method

International Nuclear Information System (INIS)

Ming, Jinfa; Liu, Zhi; Bie, Shiyu; Zhang, Feng; Zuo, Baoqi

2014-01-01

Bombyx mori silk fibroin from the silkworm was firstly found to be soluble in formic acid/hydroxyapatite system. The rheological behavior of silk fibroin solution was significantly influenced by HAp contents in dissolved solution. At the same time, silk fibroin nanofibers were observed in dissolved solution with 103.6 ± 20.4 nm in diameter. Moreover, the structure behavior of SF films prepared by formic acid/hydroxyapatite dissolution method was examined. The secondary structure of silk fibroin films was attributed to silk II structure (β-sheet), indicating that the hydroxyapatite contents in dissolved solution were not significantly affected by the structure of silk fibroin. The X-ray diffraction results exhibited obviously hydroxyapatite crystalline nature existing in silk fibroin films; however, when the hydroxyapatite content was 5.0 wt.% in dissolved solution, some hydroxyapatite crystals were converted to calcium hydrogen phosphate dehydrate in silk fibroin dissolution process. This result was also confirmed by Fourier transform infrared analysis and DSC measurement. In addition, silk fibroin films prepared by this dissolution method had higher breaking strength and extension at break. Based on these analyses, an understanding of novel SF dissolution method may provide an additional tool for designing and synthesizing advanced materials with more complex structures, which should be helpful in different fields, including biomaterial applications. - Highlights: • SF fibers were firstly successfully dissolved in FA/HAp solution. • The rheological behavior of SF solution was significantly influenced by HAp contents. • SF nanofibrils were observed in FA/HAp solution with 103.6 ± 20.4 nm in diameter. • SF films prepared by FA/HAp dissolution method had higher mechanical properties

Novel silk fibroin films prepared by formic acid/hydroxyapatite dissolution method

Energy Technology Data Exchange (ETDEWEB)

Ming, Jinfa, E-mail: jinfa.ming@gmail.com [National Engineering Laboratory for Modern Silk, Soochow University, Suzhou 215123 (China); College of Textile and Clothing Engineering, Soochow University, Suzhou 215021 (China); Liu, Zhi; Bie, Shiyu [National Engineering Laboratory for Modern Silk, Soochow University, Suzhou 215123 (China); College of Textile and Clothing Engineering, Soochow University, Suzhou 215021 (China); Zhang, Feng [Jiangsu Province Key Laboratory of Stem Cell Research, Medical College, Soochow University, Suzhou 215006 (China); Zuo, Baoqi, E-mail: bqzuo@suda.edu.cn [National Engineering Laboratory for Modern Silk, Soochow University, Suzhou 215123 (China); College of Textile and Clothing Engineering, Soochow University, Suzhou 215021 (China)

2014-04-01

Bombyx mori silk fibroin from the silkworm was firstly found to be soluble in formic acid/hydroxyapatite system. The rheological behavior of silk fibroin solution was significantly influenced by HAp contents in dissolved solution. At the same time, silk fibroin nanofibers were observed in dissolved solution with 103.6 ± 20.4 nm in diameter. Moreover, the structure behavior of SF films prepared by formic acid/hydroxyapatite dissolution method was examined. The secondary structure of silk fibroin films was attributed to silk II structure (β-sheet), indicating that the hydroxyapatite contents in dissolved solution were not significantly affected by the structure of silk fibroin. The X-ray diffraction results exhibited obviously hydroxyapatite crystalline nature existing in silk fibroin films; however, when the hydroxyapatite content was 5.0 wt.% in dissolved solution, some hydroxyapatite crystals were converted to calcium hydrogen phosphate dehydrate in silk fibroin dissolution process. This result was also confirmed by Fourier transform infrared analysis and DSC measurement. In addition, silk fibroin films prepared by this dissolution method had higher breaking strength and extension at break. Based on these analyses, an understanding of novel SF dissolution method may provide an additional tool for designing and synthesizing advanced materials with more complex structures, which should be helpful in different fields, including biomaterial applications. - Highlights: • SF fibers were firstly successfully dissolved in FA/HAp solution. • The rheological behavior of SF solution was significantly influenced by HAp contents. • SF nanofibrils were observed in FA/HAp solution with 103.6 ± 20.4 nm in diameter. • SF films prepared by FA/HAp dissolution method had higher mechanical properties.

The Effects of Silk Protein Solution on Quality of Mangosteen

International Nuclear Information System (INIS)

Phadvibulya, Valailak; Sudatis, Boonya; Panyarum, Kanyarat; Junsaithong, Mayuree; Kerdchoechuen, Orapin

2011-06-01

Full text: Sericin silk protein solution prepared from irradiated silk waste was applied as a wax coating on mangosteen fruits but was found not appropriate. Nonetheless, when the solution was sprayed onto fruits from the setting stage till maturity, it enhanced the fruit quality. Fruits showed a bigger stalk and greener, thicker and larger-angled calyx than untreated ones. They were edible after being kept at 25 C for 3 to 4 weeks. Fruits sprayed with the silk protein solution and untreated fruits were separately harvested and packed for export. A half of them were irradiated with gamma radiation for insect eradication and then kept at 10 C with 80 percents relative humidity. The unirradiated half was stored similarly. Results showed that rind color of irradiated fruits changed slower than unirradiated ones. However, silk protein solution spraying and irradiation did not affect fruit firmness and total soluble solids of mangosteen flesh. For sensory evaluation, it was found that sprayed and irradiated fruits showed no differences from the untreated ones in their physical properties, color, taste and odor. Fruits sprayed with the silk protein solution without irradiation had the longest shelf life of 6 weeks

Natural Non-Mulberry Silk Nanoparticles for Potential-Controlled Drug Release

Science.gov (United States)

Wang, Juan; Yin, Zhuping; Xue, Xiang; Kundu, Subhas C.; Mo, Xiumei; Lu, Shenzhou

2016-01-01

Natural silk protein nanoparticles are a promising biomaterial for drug delivery due to their pleiotropic properties, including biocompatibility, high bioavailability, and biodegradability. Chinese oak tasar Antheraea pernyi silk fibroin (ApF) nanoparticles are easily obtained using cations as reagents under mild conditions. The mild conditions are potentially advantageous for the encapsulation of sensitive drugs and therapeutic molecules. In the present study, silk fibroin protein nanoparticles are loaded with differently-charged small-molecule drugs, such as doxorubicin hydrochloride, ibuprofen, and ibuprofen-Na, by simple absorption based on electrostatic interactions. The structure, morphology and biocompatibility of the silk nanoparticles in vitro are investigated. In vitro release of the drugs from the nanoparticles depends on charge-charge interactions between the drugs and the nanoparticles. The release behavior of the compounds from the nanoparticles demonstrates that positively-charged molecules are released in a more prolonged or sustained manner. Cell viability studies with L929 demonstrated that the ApF nanoparticles significantly promoted cell growth. The results suggest that Chinese oak tasar Antheraea pernyi silk fibroin nanoparticles can be used as an alternative matrix for drug carrying and controlled release in diverse biomedical applications. PMID:27916946

The Effects of Silk Protein Solution on Quality of Mangosteen

Energy Technology Data Exchange (ETDEWEB)

Phadvibulya, Valailak; Sudatis, Boonya; Panyarum, Kanyarat; Junsaithong, Mayuree [Thailand Institute of Nuclear Technology, Nakhon Nayok, (Thailand); Kerdchoechuen, Orapin [School of Bioresources and Technology, King Mongkuts University, Bangkok (Thailand)

2011-06-15

Full text: Sericin silk protein solution prepared from irradiated silk waste was applied as a wax coating on mangosteen fruits but was found not appropriate. Nonetheless, when the solution was sprayed onto fruits from the setting stage till maturity, it enhanced the fruit quality. Fruits showed a bigger stalk and greener, thicker and larger-angled calyx than untreated ones. They were edible after being kept at 25{sup C} for 3 to 4 weeks. Fruits sprayed with the silk protein solution and untreated fruits were separately harvested and packed for export. A half of them were irradiated with gamma radiation for insect eradication and then kept at 10{sup C} with 80 percents relative humidity. The unirradiated half was stored similarly. Results showed that rind color of irradiated fruits changed slower than unirradiated ones. However, silk protein solution spraying and irradiation did not affect fruit firmness and total soluble solids of mangosteen flesh. For sensory evaluation, it was found that sprayed and irradiated fruits showed no differences from the untreated ones in their physical properties, color, taste and odor. Fruits sprayed with the silk protein solution without irradiation had the longest shelf life of 6 weeks.

Fluxgate magnetorelaxometry of superparamagnetic nanoparticles for hydrogel characterization

International Nuclear Information System (INIS)

Heim, Erik; Harling, Steffen; Poehlig, Kai; Ludwig, Frank; Menzel, Henning; Schilling, Meinhard

2007-01-01

A new characterization method for hydrogels based on the relaxation behavior of superparamagnetic nanoparticles (MNPs) is proposed. MNPs are incorporated in the hydrogel to examine its network properties. By analyzing their relaxation behavior, incorporated and mobile nanoparticles can be studied. In the case of mobile nanoparticles, the microviscosity of the hydrogel can be determined. Thus, this method allows the studying of gelation as well as the degradation process of hydrogels. Furthermore, the hydrogel can have any shape (e.g. microspheres or larger blocks) and no sample preparation is needed, avoiding artefacts

Orientational structure formation of silk fibroin with anisotropic properties in solutions

International Nuclear Information System (INIS)

Kholmuminov, A.A.

2008-06-01

Key words:silk fibroin, dissolution, solution's model systems, gelation, orientational crystallization, optical polarization, longitudinal stream, α - β transition, structure formation, phase transformations, relaxation, anisotropy of swelling and desorption, thermo- and biodegradation. Subjects of the inquiry: silk fibroin is the main subject of investigation. Fibroin's solutions were obtained on the base of water and organic solvents, containing salts. Comparative investigations were carried out by using biosolution - secretion of silkworm, solutions of silk sericin, cotton cellulose, methylcellulose, polystyrene and (co) polycrylonitrile. Aim of the inquiry: the elucidation of the regularities of silk fibroin anisotropic structures formation in the direct generation of orientational ordering in solutions taking into account of influences of its the molecular structures, configuration information, α - β conformational transformations, and development jointly using polarization-optical and hydrodynamic methods to control of structure formation. And also definition of possibility fields for use biopolymers anisotropic structure formation principles. Method of inquiry: birefringence, dispersion optical rotation, circular dichroism, polarization- ultramicroscope, ultracentrifuge, viscosimetry, potentiometry, differential thermal analysis, chromatography, x-ray analysis, spectroscopy. The results achieved and their novelty: the physical regularity amorphous-crystalline fibroin dissolutions in salt-containing solvents based on chains melting, distribution and redistribution were recognized; fibroin statistical parameters, molecular-mass and conformational characteristics were established; It was shown that fibroin molecules turned into fully uncoiled and oriented state with the breakdown decay of α-spiral chain sections by I type phase transition mechanism, but in oriented state with α-spiral conservation by II type transition; the presence of longitudinal field

Biodegradation of PVP-CMC hydrogel film: a useful food packaging material.

Science.gov (United States)

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.

Durable flame retardant finish for silk fabric using boron hybrid silica sol