Structure and gelation mechanism of silk hydrogels

Nagarkar, Shailesh; Nicolai, Taco; Chassenieux, Christophe; Lele, Ashish

doi:10.1039/b916319k

Cited by 92 publications

(92 citation statements)

References 34 publications

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“…Confocal Laser Scanning Microscopy (CLSM) : RSF was labeled by RITC according to Nagarkar's previous work, [ 42 ] by adding a small amount of the concentrated RITC solution to the RSF solution. The concentration of RITC in the fi nal solution was around 5 ppm.…”

Section: Methodsmentioning

confidence: 99%

Physically Crosslinked Biocompatible Silk‐Fibroin‐Based Hydrogels with High Mechanical Performance

Luo

Yang

Shao

2015

Adv Funct Materials

191

174

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have indeed shown greater mechanical performance than the traditional hydrogels. [8][9][10][11][12][13] However, problems still remained in terms of the applications of these hydrogels in biomedical fi elds. First, even if the elasticity of these hydrogels is improved signifi cantly, the modulus is far worse to meet the needs. Beyond that, poor biocompatibility as well as the possible toxicity of degradation product of these hydrogels poses a potential risk for the health of living beings. [ 6,7,14 ] Natural polymers, such as agarose, gelatin, hyaluronic acid and silk, possessing good biocompatibility, and the nontoxic degradation products, have received increasing interest in biomedical fi elds in the past decades. [ 15 ] Although these natural polymer based hydrogels have been extensively studied as the potential matrix for tissue engineering, the poor mechanical performance of the natural polymer based hydrogels is still a major limitation or a disadvantage for their medical applications. [ 16 ] Therefore, many methods were employed to improve the mechanical properties of the natural polymer based hydrogels. Chemical crosslinking was used as a facile routine approach to boost the mechanical properties of the natural polymer based hydrogels, but the safety of the chemical crosslinking reagent involved was a primary concern and the use of that might cause some unfavorable problems. [ 14 ] Besides chemical crosslinking, other efforts such as physical treatments [ 17,18 ] or mixing with other natural/synthetic polymers, [ 15,19 ] have been made to strengthen the natural polymer based hydrogels, yet the problem is still no closer to be solved.Among all natural polymers, Bombyx mori silk fi broin (SF) is one of the ideal candidates for biomedical applications due to it combining suffi cient mechanical performance, biocompatibility, and biodegradability. [20][21][22][23][24] Many approaches were employed to fabricate the physically crosslinked silk based hydrogels, such as sonication, vortex, addition of ethanol, and electrical fi eld. [25][26][27][28][29] However, most of the SF based hydrogels show poor mechanical performance which is a major stumbling block for applications. Recently, though a new covalently crosslinked SF based hydrogel with signifi cant elasticity was engineered via a kind of bio-crosslink reagent, i.e., HRP (horseradish peroxide), [ 7 ] it still could not escape the fate of poor mechanical properties in terms of the softness. Besides, the formation of the heterogeneous aggregates of crosslinking sites in the process of gelation can result in the poor optical properties Physically Crosslinked Biocompatible Silk-Fibroin-Based Hydrogels with High Mechanical PerformanceKunyuan Luo , Yuhong Yang , and Zhengzhong Shao * Developing hydrogel which combines superior mechanical performance and biocompatibility attracts researchers' attention in recent years. Here, a novel biocompatible hydrogel with excellent mechanical performance, comprised of regenerated silk fi broin (RSF) and hydroxypropyl methyl ce...

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Section: Methodsmentioning

confidence: 99%

Physically Crosslinked Biocompatible Silk‐Fibroin‐Based Hydrogels with High Mechanical Performance

Luo

Yang

Shao

2015

Adv Funct Materials

191

174

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“…As compared to other polymers, an important advantage of SF for hydrogel systems is its ability to physically crosslink without any chemical modifications. The gelation of SF is the process of protein aggregation which was related to the conformational change of the SF molecules from a random coil to β-sheet [27]. The properties of mechanical and degradation of hydrogel are largely influenced by the crystallinity and degree of physical crosslinking [28].…”

Section: Introductionmentioning

confidence: 99%

Synthesis and characterization of photocrosslinkable gelatin and silk fibroin interpenetrating polymer network hydrogels

et al. 2011

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To effectively repair or replace damaged tissues, it is necessary to design scaffolds with tunable structural and biomechanical properties that closely mimic the host tissue. In this paper, we describe a newly synthesized photocrosslinkable interpenetrating polymer network (IPN) hydrogel based on gelatin methacrylate (GelMA) and silk fibroin (SF) formed by sequential polymerization, which possesses tunable structural and biological properties. Experimental results revealed that IPNs, where both the GelMA and SF were independently crosslinked in interpenetrating networks, demonstrated a lower swelling ratio, higher compressive modulus and lower degradation rate as compared to the GelMA and semi-IPN hydrogels, where only GelMA was crosslinked. These differences were likely caused by a higher degree of overall crosslinking due to the presence of crystallized SF in the IPN hydrogels. NIH-3T3 fibroblasts readily attached to, spread, and proliferated on the surface of IPN hydrogels as demonstrated by F-actin staining and analysis of mitochondrial activity (MTT). In addition, photolithography combined with lyophilization techniques was used to fabricate 3D micropatterned and porous micro-scaffolds from GelMA-SF IPN hydrogels, furthering their versatility for use in various microscale tissue engineering applications. Overall, this study introduces a class of photocrosslinkable, mechanically robust and tunable IPN hydrogels that could be useful for various tissue engineering and regenerative medicine applications.

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“…The experiments were conducted with an X-ray diffractometer (X′ Pert-Pro MPD, PANalytical, Almelo, Holland) operating at a 40 kV tube voltage and a 40 mA tube current. CuKα radiation was used to diffract the freeze-dried gel powder with a diffraction angle 2θ = 5-45° [17][18][19][20]33] and a scanning rate of 2°/min.…”

Section: X-ray Diffraction (Xrd)mentioning

confidence: 99%

“…[17][18][19][20][30][31][32] The freeze-dried hydrogels were ground into a powder, blended with potassium bromide (KBr) and pressed into pellets prior to data collection.…”

Section: Fourier Transform Infrared (Ftir) Spectroscopic Measurementsmentioning

confidence: 99%

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Potential of biocompatible regenerated silk fibroin/sodium N-lauroyl sarcosinate hydrogels

Fang

Zhu

et al. 2015

Journal of Biomaterials Science, Polymer Edition

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Hydrogels are becoming widely used in biomaterial applications. The available methods for the preparation of these materials are continually growing. The gelation time (GT) of silk protein fibroin is difficult to control by physical methods. The cross-linkers used in available chemical techniques are likely to impact the biocompatibility of the resultant materials. In this paper, we demonstrate that the addition of sodium N-lauroyl sarcosinate (an amino-acid-based surfactant) accelerates the formation of hydrogels from fibroin. GT, turbidity variations, changes of viscoelasticity during the gelation process, and the mechanical properties of the products are measured. The secondary structure was probed by Fourier transform infrared spectroscopy, X-ray diffraction and the morphologies of the products were investigated by scanning electron microscopy. Transformations in the β-sheet content were monitored by the fluorescence of Thioflavine T and circular dichroism measurements. The relationship between the surface tension of sodium N-lauroyl sarcosinate and the GT was also explained. To investigate cell compatibility, fibroblast cells were seeded onto the surface of the hydrogels. The results indicate that the sodium N-lauroyl sarcosinate/fibroin GT can be controlled. This blend-hydrogel demonstrates excellent cell compatibility, good compression strength, and outstanding compression-recovery characteristics. Sodium N-lauroyl sarcosinate/silk fibroin hydrogels containing β-sheets have considerable potential as replacement materials in addressing the tissue defects involved with repair surgery.

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Structure and gelation mechanism of silk hydrogels

Cited by 92 publications

References 34 publications

Physically Crosslinked Biocompatible Silk‐Fibroin‐Based Hydrogels with High Mechanical Performance

Physically Crosslinked Biocompatible Silk‐Fibroin‐Based Hydrogels with High Mechanical Performance

Synthesis and characterization of photocrosslinkable gelatin and silk fibroin interpenetrating polymer network hydrogels

Potential of biocompatible regenerated silk fibroin/sodium N-lauroyl sarcosinate hydrogels

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