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Fabricating Degradable Thermoresponsive Hydrogels on Multiple Length Scales via Reactive Extrusion, Microfluidics, Self-assembly, and Electrospinning

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Photoinduced Dithiolane Crosslinking for Multiresponsive Dynamic Hydrogels.

Benjamin R Nelson^1,2, Bruce E Kirkpatrick^1,2,3, Connor E Miksch^1,2

¹Department of Chemical and Biological Engineering, University of Colorado Boulder, Boulder, CO, 80303, USA.

Advanced Materials (Deerfield Beach, Fla.)

|January 30, 2023

Summary

This summary is machine-generated.

This study introduces dithiolane photocrosslinkers for creating adaptable hydrogels. These dynamic covalent hydrogels mimic tissue properties and allow for on-demand control over mechanical and chemical characteristics.

Keywords:

dithiolanes dynamic hydrogels hyaluronic acid lipoic acid poly(ethylene glycol)

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Area of Science:

Materials Science
Biomaterials Engineering
Polymer Chemistry

Background:

Traditional hydrogels use static covalent bonds, limiting their ability to mimic dynamic biological tissues.
Viscoelastic hydrogels with adaptable crosslinks are crucial for recapitulating time- and position-dependent biological processes.

Purpose of the Study:

To present 1,2-dithiolanes as dynamic covalent photocrosslinkers for hydrogel formation.
To demonstrate the versatility of dithiolane chemistry for creating tunable hydrogels for cell-material interactions.

Main Methods:

Utilized lipoic acid as a model dithiolane for initiator-free, light-induced photopolymerization under physiological conditions.
Incorporated reversible disulfide bonds and irreversible thioether crosslinks for dynamic network control.
Employed complementary photochemical methods for rapid degradation and post-gelation stiffening.

Main Results:

Developed disulfide-crosslinked hydrogels via dithiolane photocrosslinking, enabling cell encapsulation.
Achieved multiple photoinduced dynamic responses including stress relaxation, stiffening, and softening.
Demonstrated network functionalization and tunable mechanical properties through reversible and irreversible crosslinking.

Conclusions:

Dithiolane-based hydrogel photocrosslinking offers a robust platform for adaptable biomaterials.
This chemistry allows for precise control over hydrogel properties, facilitating studies of 2D and 3D cell-material interactions.
The developed hydrogels possess a range of biologically relevant, on-demand tunable properties.