High water content silk protein-based hydrogels with tunable elasticity fabricated via a Ru(II) mediated photochemical cross-linking method

Zhang, Di; Han, Ping; Sun, Baochang; Lyu, Shanshan

doi:10.1007/s12221-017-7463-6

Cited by 14 publications

(20 citation statements)

References 41 publications

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“…Typical concentrations of Ru and APS used in dityrosine photocrosslinked hydrogels range from 100 to 1,000 µM Ru and 10 to 100 mM APS (Elvin et al, 2010;Fang and Li, 2012;Ding et al, 2013;Zhang et al, 2017;Min et al, 2018). The conversion of [Ru(II)bpy 3 ] 2+ to [Ru(II)bpy 3 ] 3+ consumes APS, thus we expect G ′ can be controlled by modulating [APS] in the crosslinking formulation.…”

Section: Targeted Hydrogel Elastic Moduli With Multiple Materials Formmentioning

confidence: 99%

“…Dityrosine photocrosslinking is an attractive and simple approach that exploits light and photoinitiator-activated phenolic coupling of tyrosyl groups within synthetic or natural polymers (Aeschbach et al, 1976;Fancy and Kodadek, 1999;Partlow et al, 2016). The photoinitiator tris(2,2 ′ -bipyridyl)ruthenium(II) ([Ru(II)bpy 3 ] 2+ ) and persulfate oxidizing agents are often used for rapid dityrosine photocrosslinking (Elvin et al, 2005(Elvin et al, , 2010Fang and Li, 2012;Ding et al, 2013;Jeon et al, 2015;Yang et al, 2015;Kim et al, 2017;Zhang et al, 2017;Min et al, 2018;Sakai et al, 2018;Khanmohammadi et al, 2019;Lim et al, 2019). [Ru(II)bpy 3 ] 2+ functions by absorbing visible light and reducing a persulfate anion to reach a higher energy state, [Ru(II)bpy 3 ] 3+ .…”

Section: Introductionmentioning

confidence: 99%

“…[Ru(II)bpy 3 ] 3+ oxidizes tyrosyl phenyl groups into free radicals that spontaneously dimerize (Nickel et al, 1994). The complete process of [Ru(II)bpy 3 ] 2+ (Ru)-mediated crosslinking occurs on the order of seconds to minutes, and the strategy has been used to form polymeric materials, such as hydrogels, with elastic moduli ranging from 6 kPa to over 100 kPa (Elvin et al, 2010;Ding et al, 2013;Zhang et al, 2017). The range of potential elastic moduli makes the technology sufficient to form biomaterials that mimic particular tissue matrices.…”

Section: Introductionmentioning

confidence: 99%

“…Despite the benefits of Ru-mediated dityrosine photocrosslinking, there is disagreement about the possible cytotoxicity of the Ru and persulfate crosslinking reagents (Annabi et al, 2017). In preparation of dityrosine photocrosslinked polymeric materials, persulfate concentrations have ranged from at least 1 to 200 mM, and Ru concentrations from 0.1 to 3 mM (Elvin et al, 2005(Elvin et al, , 2010Fang and Li, 2012;Ding et al, 2013;Jeon et al, 2015;Kim et al, 2017;Zhang et al, 2017;Min et al, 2018;Sakai et al, 2018;Khanmohammadi et al, 2019;Lim et al, 2019). Persulfates are strong oxidizing agents that can stress cell membranes and lead to an increased rate of apoptosis (Song et al, 2017).…”

Section: Introductionmentioning

confidence: 99%

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Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

et al. 2020

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Controlling mechanical properties of polymeric biomaterials, including the elastic modulus, is critical to direct cell behavior, such as proliferation and differentiation. Dityrosine photocrosslinking is an attractive and simple method to prepare materials that exhibit a wide range of elastic moduli by rapidly crosslinking tyrosyl-containing polymers. However, high concentrations of commonly used oxidative crosslinking reagents, such as ruthenium-based photoinitiators and persulfates, present cytotoxicity concerns. We found the elastic moduli of materials prepared by crosslinking an artificial protein with tightly controlled tyrosine molarity can be modulated up to 40 kPa by adjusting photoinitiator and persulfate concentrations. Formulations with various concentrations of the crosslinking reagents were able to target a similar material elastic modulus, but excess unreacted persulfate resulted in cytotoxic materials. Therefore, we identified a systematic method to prepare non-cytotoxic photocrosslinked polymeric materials with targeted elastic moduli for potential biomaterials applications in diverse fields, including tissue engineering and 3D bioprinting.

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Section: Targeted Hydrogel Elastic Moduli With Multiple Materials Formmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

et al. 2020

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“…19,20 In our previous studies, SF-based hydrogels were fabricated for immobilization of several industrially important enzymes; the immobilized enzymes displayed a wide-working pH range, as well as recyclability. 21−25 In addition, several methods have been developed to prepare SF-coated MNs. 26,27 For instance, Chen and co-workers fabricated Fe 2 O 3 /SF nanoparticles.…”

Section: Introductionmentioning

confidence: 99%

Self-Assembled Regenerated Silk Fibroin Microsphere-Embedded Fe₃O₄ Magnetic Nanoparticles for Immobilization of Zymolyase

Xiao

2019

ACS Omega

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Cytoplasm of Saccharomyces cerevisiae yeast cells contains a significant amount of desired intracellular products for both industrial utility and academic research. To recover intracellular compounds, it is necessary to break the yeast cells with high efficiency, which, under certain circumstances, requires the use of the lytic enzyme zymolyase to completely digest the cell walls. A promising strategy for zymolyase immobilization on silk fibroin (SF) was developed. SF/Fe3O4 magnetic microspheres (MMs) were constructed by solvent (ethanol)-induced self-assembly of SF surrounding Fe3O4 magnetic nanoparticles (MNs), which were synthesized by a coprecipitation method. Zymolyase was covalently bonded on the surface of the SF/Fe3O4 MMs by a photochemical cross-linking method to produce robust biocatalysts of zymolyase/SF/Fe3O4. The chemical, magnetic, and morphological properties of the MM supports and the immobilized zymolyase were investigated. Enzymolysis results demonstrated that the immobilized zymolyase showed good activity and stability for digesting yeast cell walls, and the biocatalyst can be readily recycled through convenient magnetic separation for reuse. At the optimum pH = 7.5, the immobilized zymolyase maintained 84% of the activity of the free zymolyase and retained 41% of its initial activity after four times of reuse. At unfavorable acidic pH = 4, the immobilized zymolyase retained 81% of its initial activity, while the free zymolyase showed no significant activity. Consequently, the SF/Fe3O4 MMs exhibit superior performance in terms of immobilizing enzymes, which have a good prospect in the biological application.

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Clinical Applicability of Visible Light‐Mediated Cross‐linking for Structural Soft Tissue Reconstruction

Major,

Longoni,

Simcock

et al. 2023

Advanced Science

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Visible light‐mediated cross‐linking has utility for enhancing the structural capacity and shape fidelity of laboratory‐based polymers. With increased light penetration and cross‐linking speed, there is opportunity to extend future applications into clinical spheres. This study evaluated the utility of a ruthenium/sodium persulfate photocross‐linking system for increasing structural control in heterogeneous living tissues as an example, focusing on unmodified patient‐derived lipoaspirate for soft tissue reconstruction. Freshly‐isolated tissue is photocross‐linked, then the molar abundance of dityrosine bonds is measured using liquid chromatography tandem mass spectrometry and the resulting structural integrity assessed. The cell function and tissue survival of photocross‐linked grafts is evaluated ex vivo and in vivo, with tissue integration and vascularization assessed using histology and microcomputed tomography. The photocross‐linking strategy is tailorable, allowing progressive increases in the structural fidelity of lipoaspirate, as measured by a stepwise reduction in fiber diameter, increased graft porosity and reduced variation in graft resorption. There is an increase in dityrosine bond formation with increasing photoinitiator concentration, and tissue homeostasis is achieved ex vivo, with vascular cell infiltration and vessel formation in vivo. These data demonstrate the capability and applicability of photocrosslinking strategies for improving structural control in clinically‐relevant settings, potentially achieving more desirable patient outcomes using minimal manipulation in surgical procedures.

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High water content silk protein-based hydrogels with tunable elasticity fabricated via a Ru(II) mediated photochemical cross-linking method

Cited by 14 publications

References 41 publications

Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

Self-Assembled Regenerated Silk Fibroin Microsphere-Embedded Fe₃O₄ Magnetic Nanoparticles for Immobilization of Zymolyase

Clinical Applicability of Visible Light‐Mediated Cross‐linking for Structural Soft Tissue Reconstruction

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High water content silk protein-based hydrogels with tunable elasticity fabricated via a Ru(II) mediated photochemical cross-linking method

Cited by 14 publications

References 41 publications

Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

Non-cytotoxic Dityrosine Photocrosslinked Polymeric Materials With Targeted Elastic Moduli

Self-Assembled Regenerated Silk Fibroin Microsphere-Embedded Fe3O4 Magnetic Nanoparticles for Immobilization of Zymolyase

Clinical Applicability of Visible Light‐Mediated Cross‐linking for Structural Soft Tissue Reconstruction

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Self-Assembled Regenerated Silk Fibroin Microsphere-Embedded Fe₃O₄ Magnetic Nanoparticles for Immobilization of Zymolyase