Photopolymerized dynamic hydrogels with tunable viscoelastic properties through thioester exchange

Brown, Tobin E.; Carberry, Benjamin J.; Worrell, Brady T.; Dudaryeva, Oksana; McBride, Matthew K.; Bowman, Christopher N.; Anseth, Kristi S.

doi:10.1016/j.biomaterials.2018.03.060

Cited by 153 publications

(163 citation statements)

References 37 publications

Supporting

Mentioning

156

Contrasting

Order By: Relevance

“…In addition, the effects of time-dependent mechanical properties, such as stress relaxation, on cell behavior have also been investigated on two dimensional substrates by using materials formed via non-covalent crosslinking [9, 10]. A variety of naturally-derived and synthetic polymers are used as three-dimensional cell culture substrates, typically following covalent crosslinking by photoinitiated- [11, 12], free-radical- [13], click- [14–16], or dynamic [17, 18] mechanisms to form substrates with tunable stiffness and viscoelasticity. However, changes in the weight percent (% w/v) of the polymers or degree of crosslinking may also affect the resulting polymer mesh size and transport properties of macromolecules.…”

Section: Introductionmentioning

confidence: 99%

Sequential modes of crosslinking tune viscoelasticity of cell-instructive hydrogels

2019

View full text Add to dashboard Cite

Materials that can mimic the fibrillar architecture of native extracellular matrix (ECM) while allowing for independent regulation of viscoelastic properties may serve as ideal, artificial ECM (aECM) to regulate cell functions. Here we describe an interpenetrating network of click-functionalized alginate, crosslinked with a combination of ionic and covalent crosslinking, and fibrillar collagen type I. Varying the mode and magnitude of crosslinking enables tunable stiffness and viscoelasticity, while altering neither the hydrogel’s microscale architecture nor diffusional transport of molecules with molecular weight relevant to typical nutrients. Further, appropriately timing sequential ionic and covalent crosslinking permits self-assembly of collagen into fibrillar structures within the network. Culture of human mesenchymal stem cells (MSCs) in this mechanically-tunable ECM system revealed that MSC expression of immunomodulatory markers is differentially impacted by the viscoelasticity and stiffness of the matrix. Together, these results describe and validate a novel material system for investigating how viscoelastic mechanical properties of ECM regulate cellular behavior.

show abstract

Section: Introductionmentioning

confidence: 99%

Sequential modes of crosslinking tune viscoelasticity of cell-instructive hydrogels

2019

View full text Add to dashboard Cite

show abstract

“…C2C12 cells were able to spread within gels with stress relaxation in the range of the one observed in muscle tissue (τ 1/2 ≈ 100 s), eventually fusing into multinucleated myotubes, while more elastic gels constrained cell growth. The same group proposed an alternative strategy based on thioester exchange to produce an adaptable hydrogel with dynamic crosslinking and τ 1/2 of ≈11 000 s . Although this rate of relaxation is slower than the ones reported for native tissues, these thioester gels allowed spreading and proliferation of encapsulated MSCs compared to their static controls.…”

Section: Mechanotransduction In Viscoelastic Materialsmentioning

confidence: 80%

The Plot Thickens: The Emerging Role of Matrix Viscosity in Cell Mechanotransduction

Cantini

Donnelly

Dalby

et al. 2019

Adv Healthcare Materials

View full text Add to dashboard Cite

Cell mechanotransduction is an area of intense research focus. Until now, very limited tools have existed to study how cells respond to changes in the extracellular matrix beyond, for example, mechanical deformation studies and twisting cytometry. However, emerging are a range of elastic, viscoelastic and even purely viscous materials that deform and dissipate on cellular length and timescales. This article reviews developments in these materials, typically translating from 2D model surfaces to 3D microenvironments and explores how cells interact with them. Specifically, it focuses on emerging concepts such as the molecular clutch model, how different extracellular matrix proteins engage the clutch under viscoelastic‐stress relaxation conditions, and how mechanotransduction can drive transcriptional control through regulators such as YAP/TAZ.

show abstract

“…However, there is no doubt about the existence of ionic interaction among the constitutional macromolecular components (G, CH, and HEC) of the hydrogels. Besides the higher stiffness and strength, the anisotropic hydrogels, particularly, G/PEG/CH (1) and G/PEG/CH (2), presented in this work showed superior stress‐relaxation response compared to other covalently crosslinked hydrogels reported in literatures …”

Section: Resultsmentioning

confidence: 99%

Rational Design and Development of Anisotropic and Mechanically Strong Gelatin‐Based Stress Relaxing Hydrogels for Osteogenic/Chondrogenic Differentiation

Dey

Agnelli

et al. 2019

Macromolecular Bioscience

View full text Add to dashboard Cite

Rational design and development of tailorable simple synthesis process remains a centerpiece of investigational efforts toward engineering advanced hydrogels. In this study, a green and scalable synthesis approach is developed to formulate a set of gelatin‐based macroporous hybrid hydrogels. This approach consists of four sequential steps starting from liquid‐phase pre‐crosslinking/grafting, unidirectional freezing, freeze‐drying, and finally post‐curing process. The chemical crosslinking mainly involves between epoxy groups of functionalized polyethylene glycol and functional groups of gelatin both in liquid and solid state. Importantly, this approach allows to accommodate different polymers, chitosan or hydroxyethyl cellulose, under identical benign condition. Structural and mechanical anisotropy can be tuned by the selection of polymer constituents. Overall, all hydrogels show suitable structural stability, good swellability, high porosity and pore interconnectivity, and maintenance of mechanical integrity during 3‐week‐long hydrolytic degradation. Under compression, hydrogels exhibit robust mechanical properties with nonlinear elasticity and stress‐relaxation behavior and show no sign of mechanical failure under repeated compression at 50% deformation. Biological experiment with human bone marrow mesenchymal stromal cells (hMSCs) reveals that hydrogels are biocompatible, and their physicomechanical properties are suitable to support cells growth, and osteogenic/chondrogenic differentiation, demonstrating their potential application for bone and cartilage regenerative medicine toward clinically relevant endpoints.

show abstract

Photopolymerized dynamic hydrogels with tunable viscoelastic properties through thioester exchange

Cited by 153 publications

References 37 publications

Sequential modes of crosslinking tune viscoelasticity of cell-instructive hydrogels

Sequential modes of crosslinking tune viscoelasticity of cell-instructive hydrogels

The Plot Thickens: The Emerging Role of Matrix Viscosity in Cell Mechanotransduction

Rational Design and Development of Anisotropic and Mechanically Strong Gelatin‐Based Stress Relaxing Hydrogels for Osteogenic/Chondrogenic Differentiation

Contact Info

Product

Resources

About