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Dual-crosslinkable gallol bioinks via pH-controlled oxidation and photocrosslinking with enhanced shear thinning and viscoelastic behavior

Lookup NU author(s): Hatai JongprasitkulORCiD, Professor David FultonORCiD

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).

Abstract

© 2025 The Authors. Our research work proposes a dual crosslinking approach to address the limitations of the gallol-mediated auto-oxidation approach in bioprinting, where rapid oxidative crosslinking can cause premature gelation, leading to clogging or printing failure. We enabled a gallol hydrogel ink to be printable via extrusion-based 3D bioprinting by utilizing its temporal shear-thinning properties. By raising the pH level, interactions between gallol-modified hyaluronic acid methacrylate (HAMA-GA) can be triggered to form a weak hydrogel. This feature provides injectability and extrudability for the hydrogels. Subsequent photocrosslinking results in indefinite oxidative crosslinking. The oxidative coupling in HAMA-GA was partially inhibited by UV light during the photocrosslinking step. As a result, the printed hydrogel formed a dual-crosslinked network containing both oxidative and photo-induced bonds, which contributed to enhanced structural stability over time. Our proposed approach addresses the challenges of gallol-mediated oxidation, including overgelation that hinders extrusion in 3D bioprinting, offering a promising solution for improved printability and shape fidelity. HAMA-GA ink was bioprintable at pH 5.5 using an extrusion-based 3D printer, showing cytocompatibility (∼95 % viability). This strategy is valuable for designing hydrogel inks with tunable properties for 3D bioprinting while maintaining tissue adhesive properties of gallol moieties.

Publication metadata

Author(s): Jongprasitkul H, Turunen S, Fulton DA, Kellomaki M, Parihar VS

Publication type: Article

Publication status: Published

Journal: Bioprinting

Year: 2025

Volume: 50

Print publication date: 01/10/2025

Online publication date: 14/08/2025

Acceptance date: 11/08/2025

Date deposited: 01/09/2025

ISSN (electronic): 2405-8866

Publisher: Elsevier BV

URL: https://doi.org/10.1016/j.bprint.2025.e00432

DOI: 10.1016/j.bprint.2025.e00432

Data Access Statement: Data will be made available on request.

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