Semiconvertible Hyaluronic Hydrogel Enabled Red-Light-Responsive Reversible Mechanics, Adhesion, and Self-Healing

Biomacromolecules. 2022 Mar 14;23(3):1030-1040. doi: 10.1021/acs.biomac.1c01395. Epub 2022 Jan 14.

Abstract

Photoresponsive supramolecular hydrogels based on the host-guest interaction between cyclodextrin (CD) and azobenzene (Azo) are highly favored in "on-demand" biological applications. Nevertheless, most Azo/CD-based hydrogels are UV-responsive, exhibiting poor tissue penetrability and potential cytotoxicity; more importantly, the complete gel-sol transition under irradiation makes intelligent systems unstable. Here, we report a red-light-responsive semiconvertible hydrogel based on tetra-ortho-methoxy-substituted Azo (mAzo)- and CD-functionalized hyaluronic acid (HA). By integrating red-shifted-photoisomerized mAzo with HA, a biocompatible 625 nm-light-responsive polymeric guest with strengthened hydrogen bonding and weakened photoisomerization was synthesized. Upon alternating irradiation, mAzo-HA/CD-HA hydrogels obtained here exhibited reversible mechanical and structural dynamics, while avoiding complete gel-sol transition. This improved semiconvertibility remedies the lack of macroscopic resilience for dynamic system so as to endow supramolecular hydrogels with spatial-temporal mechanics, self-healing, and adhesion. Together with excellent cytocompatibility and manufacturability, these hydrogels show potential advantages in tissue engineering, especially for the regeneration of functional multi-tissue complex.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cyclodextrins* / chemistry
  • Hyaluronic Acid
  • Hydrogels* / chemistry
  • Light
  • Polymers / chemistry

Substances

  • Cyclodextrins
  • Hydrogels
  • Polymers
  • Hyaluronic Acid