Journal
BIOCONJUGATE CHEMISTRY
Volume 29, Issue 4, Pages 905-913Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.bioconjchem.7b00802
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Funding
- Burroughs Wellcome Fund PDEP program [1013981]
- CASI award [1015895]
- American Heart Association
- Center for Engineering MechanoBiology from the National Science Foundation's STC program [CMMI: 15-48571]
- National Science Foundation [DMR 1408955]
- NATIONAL INSTITUTE OF DENTAL & CRANIOFACIAL RESEARCH [R01DE016523] Funding Source: NIH RePORTER
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Biomimetic hydrogels fabricated from biologically derived polymers, such as hyaluronic acid (HA), are useful for numerous biomedical applications. Due to the dynamic nature of biological processes, it is of great interest to synthesize hydrogels with dynamically tunable network properties where various functions (e.g., cargo delivery, mechanical signaling) can be changed over time. Among the various stimuli developed to control hydrogel properties, light stands out for its exquisite spatiotemporal control; however, most light-based chemistries are unidirectional in their ability to manipulate network changes. Here, we report a strategy to reversibly modulate HA hydrogel properties with light, using supra molecular cross-links formed via azobenzene bound to beta-cyclodextrin. Upon isomerization with 365 nm or 400-500 nm light, the binding affinity between azobenzene and beta-cyclodextrin changed and altered the network connectivity. The hydrogel mechanical properties depended on both the azobenzene modification and isomeric state (lower for cis state), with up to a 60% change in storage modulus with light exposure. Furthermore, the release of a fluorescently labeled protein was accelerated with light exposure under conditions that were cytocompatible to encapsulated cells. These results indicate that the developed hydrogels may be suitable for applications in which temporal regulation of material properties is important, such as drug delivery or mechanobiology studies.
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