A new boronate ester-based crosslinking strategy allows the design of nonswelling and long-term stable dynamic covalent hydrogels. (8th February 2023)

• Record Type: Journal Article
• Authors: Lagneau, N.; Terriac, L.; Tournier, P.; Helesbeux, J-J.; Viault, G.; Séraphin, D.; Halgand, B.; Loll, F.; Garnier, C.; Jonchère, C.; Rivière, M.; Tessier, A.; Lebreton, J.; Maugars, Y.; Guicheux, J.; Le Visage, C.; Delplace, V.
• Is Part Of: Biomaterials science. Volume 11:Number 6(2023)
• Page Start: 2033
• Page End: 2045
• Publication Date: 2023-02-08
• Subjects: Biomedical materials -- Periodicals; 610.28
• DOI: 10.1039/d2bm01690g
• Languages: English
• ISSNs: 2047-4830

Abstract

Abstract : Testing libraries of phenylboronic acid derivatives and diols revealed a new crosslinking couple for the formation of viscoelastic hydrogels with tunable properties and long-term stability. Abstract : Dynamic hydrogels are viscoelastic materials that can be designed to be self-healing, malleable, and injectable, making them particularly interesting for a variety of biomedical applications. To design dynamic hydrogels, dynamic covalent crosslinking reactions are attracting increasing attention. However, dynamic covalent hydrogels tend to swell, and often lack stability. Boronate ester-based hydrogels, which result from the dynamic covalent reaction between a phenylboronic acid (PBA) derivative and a diol, are based on stable precursors, and can therefore address these limitations. Yet, boronate ester formation hardly occurs at physiological pH. To produce dynamic covalent hydrogels at physiological pH, we performed a molecular screening of PBA derivatives in association with a variety of diols, using hyaluronic acid as a polymer of interest. The combination of Wulff-type PBA (wPBA) and glucamine stood out as a unique couple to obtain the desired hydrogels. We showed that optimized wPBA/glucamine hydrogels are minimally- to non-swelling, stable long term (over months), tunable in terms of mechanical properties, and cytocompatible. We further characterized their viscoelastic and self-healing properties, highlighting their potential for biomedical applications.