Hybrid Vesicles Enable Mechano-Responsive Hydrogel Degradation

Sung-Won Hwang; Chung-Man Lim; Cong Truc Huynh; Hossein Moghimianavval; Nicholas A Kotov; Eben Alsberg; Allen P Liu

doi:10.1002/anie.202308509

Hybrid Vesicles Enable Mechano-Responsive Hydrogel Degradation

Angew Chem Int Ed Engl. 2023 Oct 9;62(41):e202308509. doi: 10.1002/anie.202308509. Epub 2023 Sep 4.

Authors

Sung-Won Hwang¹, Chung-Man Lim², Cong Truc Huynh³, Hossein Moghimianavval⁴, Nicholas A Kotov^{1

2

5}, Eben Alsberg^{3

6}, Allen P Liu^{4

7}

Affiliations

¹ Department of Chemical Engineering, University of Michigan, Ann Arbor, MI, 48109, USA.
² Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, 48109, USA.
³ Department of Biomedical Engineering, University of Illinois Chicago, Chicago, IL, 60612, USA.
⁴ Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI, 48109, USA.
⁵ Departments of Biomedical Engineering, Macromolecular Science and Engineering, Biointerfaces Institute, University of Michigan, Ann Arbor, MI, 48109, USA.
⁶ Departments of Orthopedic Surgery, Pharmacology and Regenerative Medicine, and Mechanical and Industrial Engineering, University of Illinois Chicago, Chicago, IL, 60612, USA.
⁷ Departments of Biomedical Engineering, Biophysics, Cellular and Molecular Biology Program, Applied Physics Program, University of Michigan, Ann Arbor, MI, 48109, USA.

PMID: 37607024
PMCID: PMC10600738 (available on 2024-10-09)
DOI: 10.1002/anie.202308509

Abstract

Stimuli-responsive hydrogels are intriguing biomimetic materials. Previous efforts to develop mechano-responsive hydrogels have mostly relied on chemical modifications of the hydrogel structures. Here, we present a simple, generalizable strategy that confers mechano-responsive behavior on hydrogels. Our approach involves embedding hybrid vesicles, composed of phospholipids and amphiphilic block copolymers, within the hydrogel matrix to act as signal transducers. Under mechanical stress, these vesicles undergo deformation and rupture, releasing encapsulated compounds that can control the hydrogel network. To demonstrate this concept, we embedded vesicles containing ethylene glycol tetraacetic acid (EGTA), a calcium chelator, into a calcium-crosslinked alginate hydrogel. When compressed, the released EGTA sequesters calcium ions and degrades the hydrogel. This study provides a novel method for engineering mechano-responsive hydrogels that may be useful in various biomedical applications.

Keywords: Block Copolymers; Functional Material; Stimuli-Responsive Hydrogel; Stress-Induced Degradation; Vesicles.

Abstract

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