Structure–Chemical Modification Relationships with Silk Materials

Ma, Jiachi; Liu, Siyuan; Zhang, Xiaoyi; Liu, Bing; Ding, Zhaozhao; Lü, Qiang; Chen, Hong; Kaplan, David L.

doi:10.1021/acsbiomaterials.9b00369

Cited by 18 publications

(30 citation statements)

References 65 publications

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“…Both FTIR and XRD spectra of SNF indicated similar conformations to SF, suggesting the amorphous state of SNFs in aqueous solution (Figure B,C). The deconvolution of amide I (Table S1, Supporting Information) further confirmed the similar secondary structures of SF and SNF where the beta sheet ratios were 28.03 ± 2.77% and 29.17 ± 3.29%, respectively . Compared to that of SF (−30 mv), SNFs showed significantly lower Zeta potential (−7 mv), which revealed their various group distributions among the two solution systems.…”

Section: Resultssupporting

confidence: 52%

“…The different secondary conformations and HRP crosslinking resulted in different degradation behaviors (Figure S2A,B, Supporting Information). Although the β‐sheet content of the silk nanofiber hydrogels (SNF1, SNF2, SNF3) was slightly higher than that of SF2 hydrogels (Table S1, Supporting Information), the nanofiber hydrogels showed significantly slower degradation partly due to their higher crosslinking density . SNF1 hydrogels with highest β‐sheet content degraded more quickly than SNF2 and SNF4 with lower β‐sheet structure, further suggesting the stabilization capacity of crosslinking.…”

Section: Resultsmentioning

confidence: 97%

“…The samples were analyzed with Nicolet FTIR 5700 spectrometer (Thermo Scientific, FL, U.S.A.) from 1800 to 1400 cm −1 . The amide I region was deconvolved through PeakFit software to calculate the contents of the secondary conformations . The crystal structure of the samples was measured with X‐ray diffraction (XRD, Nano ZS90, Malvern, Instruments, Malvern, U.K.).…”

Section: Methodsmentioning

confidence: 99%

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Amorphous Silk Fibroin Nanofiber Hydrogels with Enhanced Mechanical Properties

Liu

Ding

et al. 2019

Macromolecular Bioscience

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Silk fibroin (SF) hydrogels have been engineered as universal substrates for various tissue regenerations and drug delivery. Although different physical and chemical crosslinking strategies are developed to form SF hydrogels with suitable performances, a significant gap remains to match specific requirements of various tissues. Here, amorphous SF nanofibers with more tyrosine residues outside the surfaces are used to replace traditional SF. Under the same crosslinking conditions, the use of amorphous SF nanofibers results in tougher properties, four times higher stiffness than that from traditional SF solutions. Unlike previous SF hydrogels, the SF nanofiber hydrogels show high tunability in wide modulus range of 0.6–160 kPa under low SF concentrations (below 5 wt%), showing improved mechanical match with various soft tissues. Better stability and cytocompatibility are also achieved, further confirming the superiority of the hydrogels as the tissue substrates. Therefore, a feasible strategy is developed to optimize the performances of SF hydrogel via tuning the nano‐structural state in aqueous solutions, which will enrich SF‐based hydrogel family in future.

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Section: Resultssupporting

confidence: 52%

Section: Resultsmentioning

confidence: 97%

Section: Methodsmentioning

confidence: 99%

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Amorphous Silk Fibroin Nanofiber Hydrogels with Enhanced Mechanical Properties

Liu

Ding

et al. 2019

Macromolecular Bioscience

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“…The observation of SEM showed that interconnected microstructures with regular sheeted-shape were detected ( Figure 4 ). These results demonstrated that dialysis periods affect the formation with microstructures and interconnection of these structures with sheeted-shape through the elimination of strong salt and unreacted chemicals [ 24 , 25 , 26 ].…”

Section: Resultsmentioning

confidence: 99%

Cytocompatibility of Modified Silk Fibroin with Glycidyl Methacrylate for Tissue Engineering and Biomedical Applications

Hong

Lee

et al. 2020

Biomolecules

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Hydrogel with chemical modification has been used for 3D printing in the biomedical field of cell and tissue-based regeneration because it provides a good cellular microenvironment and mechanical supportive ability. As a scaffold and a matrix, hydrogel itself has to be modified chemically and physically to form a β-sheet crosslinking structure for the strength of the biomaterials. These chemical modifications could affect the biological damage done to encapsulated cells or surrounding tissues due to unreacted chemical residues. Biological assessment, including assessment of the cytocompatibility of hydrogel in clinical trials, must involve testing with cytotoxicity, irritation, and sensitization. Here, we modified silk fibroin and glycidyl methacrylate (Silk-GMA) and evaluated the physical characterizations, residual chemical detection, and the biological effect of residual GMA depending on dialysis periods. Silk-GMA depending on each dialysis period had a typical β-sheet structure in the characterization analysis and residual GMA decreased from dialysis day 1. Moreover, cell proliferation and viability rate gradually increased; additionally, necrotic and apoptotic cells decreased from dialysis day 2. These results indicate that the dialysis periods during chemical modification of natural polymer are important for removing unreacted chemical residues and for the potential application of the manufacturing standardization for chemically modified hydrogel for the clinical transplantation for tissue engineering and biomedical applications.

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“…[ 9,10 ] With design strategies for supramolecular structures in place, more research is now being conducted that explores the accessibility and reactivity of these supramolecular surfaces to expand the potential applications of peptide‐based biomaterials. [ 11–13 ]…”

Section: Introductionmentioning

confidence: 99%

Modifying the surface of peptide nanofibers utilizing a thiol‐thioester exchange

et al. 2020

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Herein, we report on the incorporation of a dithioester modification to a self‐assembling peptide and characterize a thiol‐thioester exchange on the nanofiber's surface with respect to amount of soluble exogenous thiol present and pH of the reaction. The ratios of all peptide species throughout the exchange reaction were reproducibly monitored by matrix‐assisted laser desorption ionization time‐of‐flight (MALDI‐TOF) mass spectrometry, highlighting the utility of MALDI to characterize heterogeneous and dynamic supramolecular systems. The tuneable revealing of thiols through a dynamic covalent chemical reaction presents a new strategy for labeling supramolecular surfaces. This strategy of combining reversible peptide self‐assembly and dynamic covalent chemistry opens another route for the post‐assembly modification of amyloid‐based supramolecular structures and the design of functional biomaterials.

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Structure–Chemical Modification Relationships with Silk Materials

Cited by 18 publications

References 65 publications

Amorphous Silk Fibroin Nanofiber Hydrogels with Enhanced Mechanical Properties

Amorphous Silk Fibroin Nanofiber Hydrogels with Enhanced Mechanical Properties

Cytocompatibility of Modified Silk Fibroin with Glycidyl Methacrylate for Tissue Engineering and Biomedical Applications

Modifying the surface of peptide nanofibers utilizing a thiol‐thioester exchange

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