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Dynamic Supramolecular Hydrogels Spanning an Unprecedented Range of Host–Guest Affinity
- Zou, Lei, Braegelman, Adam S., Webber, Matthew J.
- ACS applied materials & interfaces 2019 v.11 no.6 pp. 5695-5700
- binding capacity, crosslinking, encapsulation, hydrogels, macrocyclic compounds, materials science
- Cucurbituril (CB) macrocycles exhibit a broad range of host–guest binding affinity. Attaching pendant CB and complementary guests on 8-arm PEG macromers affords supramolecular hydrogels with cross-link affinity spanning more than 5 orders of magnitude (1.5 × 10⁷ to 5.4 × 10¹² M–¹) without changing network topology. Cross-link affinity translates directly to bulk dynamic properties; hydrogels with high-affinity cross-linking behave like covalent gels with limited ability to relax or self-heal. Cross-link affinity furthermore dictates the release rate of encapsulated macromolecules, as well as cell infiltration and material clearance in vivo. This work thus informs a role for affinity in dictating supramolecular hydrogel properties by quantifying and isolating this feature over an unprecedented range.