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Self-Aggregation-Induced Polymerization for Constructing Multifunctional Dynamic Zwitterionic Hydrogels
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DOI：10.1002/agt2.70227.png)
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Abstract
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Zwitterionic hydrogels have attracted considerable attention as advanced biomaterials. However, the fabrication of traditional zwitterionic hydrogels typically relies on harsh polymerization conditions, and their backbone structures are non-biodegradable. In this study, we develop a self-aggregation-induced polymerization (SAIP) mechanism that enables the spontaneous formation of multifunctional zwitterionic hydrogels under mild aqueous conditions, utilizing a rationally designed lipoic acid-carboxybetaine monomer with lipoic acid-modified hyaluronic acid (LAHA) crosslinker. This SAIP mechanism is driven by the synergistic interaction between the strongly hydrophilic zwitterionic moieties and hydrophobic 1,2-dithiolanes, promoting monomer self-aggregation into high-concentration reactive microenvironments, thus facilitating efficient ring-opening polymerization without external catalysts or stimuli. The incorporation of LAHA as a crosslinker results in the formation of a stable zwitterionic hydrogel, distinguished by its mild preparation conditions, rapid spontaneous gelation (116 s), and controlled depolymerization through dynamic disulfide bonds. Furthermore, the resulting hydrogel demonstrates high water content (>76%), robust mechanical properties (compressive stress up to 3.86 MPa), exceptional antioxidant activity (>90% DPPH scavenging), high biocompatibility, and superior living cell encapsulation and protection. This study provides a fundamental understanding of hydrogel formation through the SAIP mechanism and advances the development of zwitterionic hydrogels, making the resulting hydrogel an attractive candidate for biomedical applications.
Keywords:
antioxidant activity
dynamic hydrogel network
living cell encapsulation
self-aggregation-induced polymerization
zwitterionic hydrogel
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