Enzymatically crosslinked silk-hyaluronic acid hydrogels

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

doi:10.1016/j.biomaterials.2017.03.046

Cited by 246 publications

(195 citation statements)

References 69 publications

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“…For cell encapsulation purposes, this might cause uneven cell distribution and leaves cells exposed to H 2 O 2 , which can result in cellular damage and low viability . Moreover, these hydrogels undergo a spontaneous random coil to β‐sheet transition, causing a gradual increase in hydrogel stiffness over time . Unless specifically desired, this 10–100‐fold increase in stiffness over time makes the enzymatically crosslinked hydrogels unpredictable constructs for regenerative medicine applications.…”

Section: Introductionmentioning

confidence: 99%

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Rapid Photocrosslinking of Silk Hydrogels with High Cell Density and Enhanced Shape Fidelity

Cui

Soliman

Alcala-Orozco

et al. 2020

Adv Healthcare Materials

121

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Silk fibroin hydrogels crosslinked through di‐tyrosine bonds are clear, elastomeric constructs with immense potential in regenerative medicine applications. In this study, demonstrated is a new visible light‐mediated photoredox system for di‐tyrosine bond formation in silk fibroin that overcomes major limitations of current conventional enzymatic‐based crosslinking. This photomediated system rapidly crosslinks silk fibroin (<1 min), allowing encapsulation of cells at significantly higher cell densities (15 million cells mL−1) while retaining high cell viability (>80%). The photocrosslinked silk hydrogels present more stable mechanical properties which do not undergo spontaneous transition to stiff, β‐sheet‐rich networks typically seen for enzymatically crosslinked systems. These hydrogels also support long‐term culture of human articular chondrocytes, with excellent cartilage tissue formation. This system also facilitates the first demonstration of biofabrication of silk fibroin constructs in the absence of chemical modification of the protein structure or rheological additives. Cell‐laden constructs with complex, ordered, graduated architectures, and high resolution (40 µm) are fabricated using the photocrosslinking system, which cannot be achieved using the enzymatic crosslinking system. Taken together, this work demonstrates the immense potential of a new crosslinking approach for fabrication of elastomeric silk hydrogels with applications in biofabrication and tissue regeneration.

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Section: Introductionmentioning

confidence: 99%

“…Moreover, these hydrogels undergo a spontaneous random coil to β‐sheet transition, causing a gradual increase in hydrogel stiffness over time . Unless specifically desired, this 10–100‐fold increase in stiffness over time makes the enzymatically crosslinked hydrogels unpredictable constructs for regenerative medicine applications.…”

Section: Introductionmentioning

confidence: 99%

Rapid Photocrosslinking of Silk Hydrogels with High Cell Density and Enhanced Shape Fidelity

Cui

Soliman

Alcala-Orozco

et al. 2020

Adv Healthcare Materials

121

View full text Add to dashboard Cite

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“…201 Due to the mild reaction conditions, enzyme-catalyzed reactions have gained increasing popularity for hydrogel synthesis. 82 Various enzymes, including horseradish peroxidase (HRP), 202, 203 transglutaminase (Factor XIII), 83, 204 tyrosinase (Tyr), 205, 206 phosphopantetheinyl transferase (PPTase), 207 lysyl oxidase 208 and phosphatases 209, 210 have been explored to catalyze gelation. For example, using PEG-based microgels with a uniform size and displaying transglutaminase peptide substrates K and Q, Griffin et al produced a microporous gel via FXIIIa-catalyzed amide formation between the K and Q peptides.…”

Section: Chemical Approaches To Hydrogel Synthesismentioning

confidence: 99%

Chemical synthesis of biomimetic hydrogels for tissue engineering

2017

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Owing to the high water content, porous structure, biocompatibility and tissue-like viscoelasticity, hydrogels have become attractive and promising biomaterials for use in drug delivery, 3D cell culture and tissue engineering applications. Various chemical approaches have been developed for hydrogel synthesis using monomers or polymers carrying reactive functional groups. For in vivo tissue repair and in vitro cell culture purposes, it is desirable that the crosslinking reactions occur under mild conditions, do not interfere with biological processes and proceed at high yield with exceptional selectivity. Additionally, the cross-linking reaction should allow straightforward incorporation of bioactive motifs or signaling molecules, at the same time, providing tunability of the hydrogel microstructure, mechanical properties, and degradation rates. In this review, we discuss various chemical approaches applied to the synthesis of complex hydrogel networks, highlighting recent developments from our group. The discovery of new chemistries and novel materials fabrication methods will lead to the development of the next generation biomimetic hydrogels with complex structures and diverse functionalities. These materials will likely facilitate the construction of engineered tissue models that may bridge the gap between 2D experiments and animal studies, providing preliminary insight prior to in vivo assessments.

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“…HA, an essential component of extra cellular matrix, is well known for its hydrophilic and water retaining properties5 and considered to be one of the key components of the wound healing process, modulating inflammation, cellular migration, and angiogenesis 6. With the aforementioned physical and physiological properties, HA‐based hydrogel wound dressings can serve a dual function as active drug carriers and wound healing agents.…”

Section: Introductionmentioning

confidence: 99%

Development of Biocompatible HA Hydrogels Embedded with a New Synthetic Peptide Promoting Cellular Migration for Advanced Wound Care Management

et al. 2018

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In the past few years, there have been many efforts underway to develop effective wound healing treatments for traumatic injuries. In particular, wound‐healing peptides (WHPs) and peptide‐grafted dressings hold great promise for novel therapeutic strategies for wound management. This study reports a topical formulation of a new synthetic WHP (REGRT, REG) embedded in a hyaluronic acid (HA)‐based hydrogel dressing for the enhancement of acute excisional wound repair. The copper‐free click chemistry is utilized to form biocompatible HA hydrogels by cross‐linking dibenzocyclooctyl‐functionalized HA with 4‐arm poly(ethylene glycol) (PEG) azide. The HA hydrogels are grafted with the REG peptide, a functional derivative of erythroid differentiation regulator1, displaying potent cell motility‐stimulating ability, thus sustainably releasing physiologically active peptides for a prolonged period. Combined with the traditional wound healing benefits of HA, the HA hydrogel embedded REG (REG‐HAgel) accelerates re‐epithelialization in skin wound healing, particularly by promoting migration of fibroblasts, keratinocytes, and endothelial cells. REG‐HAgels improve not only rate, but quality of wound healing with higher collagen deposition and more microvascular formation while being nontoxic. The peptide‐grafted HA hydrogel system can be considered as a promising new wound dressing formulation strategy for the treatment of different types of wounds with combinations of various natural and synthetic WHPs.

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Enzymatically crosslinked silk-hyaluronic acid hydrogels

Cited by 246 publications

References 69 publications

Rapid Photocrosslinking of Silk Hydrogels with High Cell Density and Enhanced Shape Fidelity

Rapid Photocrosslinking of Silk Hydrogels with High Cell Density and Enhanced Shape Fidelity

Chemical synthesis of biomimetic hydrogels for tissue engineering

Development of Biocompatible HA Hydrogels Embedded with a New Synthetic Peptide Promoting Cellular Migration for Advanced Wound Care Management

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