Photochemical Control of Network Topology in PEG Hydrogels
Hydrogels are often synthesized through photoinitiated step-, chain-, and mixed-mode polymerizations, generating diverse network topologies and resultant material properties that depend on the underlying network connectivity. While many photocrosslinking reactions are available, few afford controllable connectivity of the hydrogel network. Herein, a versatile photochemical strategy is introduced for tuning the structure of poly(ethylene glycol) (PEG) hydrogels using macromolecular monomers functionalized with maleimide and styrene moieties. Hydrogels are prepared along a gradient of topologies by varying the ratio of step-growth (maleimide dimerization) to chain-growth (maleimide-styrene alternating copolymerization) network-forming reactions. The initial PEG content and final network physical properties (e.g., modulus, swelling, diffusivity) are tailored in an independent manner, highlighting configurable gel mechanics and reactivity. These photochemical reactions allow high-fidelity photopatterning and 3D printing and are compatible with 2D and 3D cell culture. Ultimately, this photopolymer chemistry allows facile control over network connectivity to achieve adjustable material properties for broad applications.
Authors
- Lea Pearl Hibbard (ORCID: https://orcid.org/0009-0008-3495-9339)
- Jason A. Burdick (ORCID: https://orcid.org/0000-0002-2006-332X)
- Connor E. Miksch (ORCID: https://orcid.org/0000-0003-0082-4862)
- Sean P. Keyser (ORCID: https://orcid.org/0000-0002-3821-6291)
- Laura J. Macdougall (ORCID: https://orcid.org/0000-0002-6255-4223)
- Timothy J. White (ORCID: https://orcid.org/0000-0001-8006-7173)
- Jasmine Sinha (ORCID: https://orcid.org/0000-0001-8396-1322)
- Christopher N. Bowman (ORCID: https://orcid.org/0000-0001-8458-7723)
- Tayler S. Hebner (ORCID: https://orcid.org/0000-0003-2723-3835)
- Bruce E. Kirkpatrick (ORCID: https://orcid.org/0000-0003-2862-3843)
- Benjamin R. Nelson (ORCID: https://orcid.org/0000-0002-6702-079X)
- Abhishek P. Dhand (ORCID: https://orcid.org/0000-0002-1470-1081)
- Benjamin D. Fairbanks
- Grace K. Hach (ORCID: https://orcid.org/0009-0009-0926-4591)
- Nathaniel P. Skillin (ORCID: https://orcid.org/0000-0003-1424-9037)
- Joshua T. Kamps (ORCID: https://orcid.org/0000-0002-3539-0227)
- Joshua S. Lee (ORCID: https://orcid.org/0000-0003-4945-5703)
- Violeta Salazar
- Henry S. Grotheer
- Kristi S. Anseth (ORCID: https://orcid.org/0000-0002-5725-5691)
Institutions
- University of Colorado Boulder (US)
- University of Colorado Anschutz Medical Campus (US)
- University of Pennsylvania (US)
Publication Details
- Journal
- Advanced Materials
- Published
- 2024-09-28
- DOI
- https://doi.org/10.1002/adma.202409603
- Citations
- 22
- Primary Topic
- Hydrogels: synthesis, properties, applications
- Type
- article
- Field-Weighted Citation Impact
- 3.75
Funders
- National Institutes of Health
- National Institute of Standards and Technology
- Defense Advanced Research Projects Agency
- National Institute of Dental and Craniofacial Research
- Defense Sciences Office, DARPA