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Heterogeneous polymerization via two-step crosslinking for tunable microribbon hydrogels
Journal article   Open access   Peer reviewed

Heterogeneous polymerization via two-step crosslinking for tunable microribbon hydrogels

Mahsa Karimi, Fereshteh Ahadi, Niloofar Esmati, Mingyue Fan, Lin Han, Christopher Y Li and Li-Hsin Han
Biofabrication, v 18(1), 015016
17 Dec 2025
DOI: https://doi.org/10.1088/1758-5090/ae235a
PMID: 41285045
Featured in Collection :   Research Supported by Drexel Libraries' OA Programs
url
https://doi.org/10.1088/1758-5090/ae235aView
Published, Version of Record (VoR)Open Access via Drexel Libraries Read and Publish Program 2025CC BY V4.0,  Open

Abstract

Heterogeneous hydrogel Porous hydrogel Multi-step crosslinking Building blocks Hydrogel polymerization Tissue Engineering
Hydrogels are widely used in tissue engineering but conventional homogeneous polymerization often creates dense matrices that hinder cell migration and restrict extracellular matrix production. The motivation of this project was to overcome these limitations by developing a heterogeneously crosslinkable hydrogel platform that enables both cell migration and matrix deposition. We present a two-step heterogeneous polymerization approach that introduces spatial variations in matrix density, producing tunable, cell-sized pores that promote migration, proliferation, and matrix synthesis. As an implementation, gelatin was pre-assembled into microribbon-like building blocks using a Dynamic Molding process, methacrylated to introduce crosslinkable groups, chemically modified, washed, and freeze-dried. Upon rehydration, the ribbons formed a moldable paste that could be mixed with cells and photo-crosslinked into scaffolds with in situ-formed, cell-sized pores. The main novelty of this method is the introduction of chemical modifications with methacrylic anhydride (MAA), acetic anhydride (AceA), and succinic anhydride (SucA), which enable a controlled two-step heterogeneous polymerization and allow independent tuning of scaffold microstructure, mechanics, and degradation. AceA reduced crosslink density and accelerated degradation, whereas SucA promoted swelling, enhanced mechanical strength, and slowed degradation. Cell studies revealed that SucA-modified scaffolds supported superior adhesion and proliferation compared to AceA-modified and unmodified controls. Such work may significantly impact the design of next-generation scaffolds by providing a versatile platform that integrates structural, mechanical, and biochemical control for regenerative medicine applications.

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Web of Science research areas
Engineering, Biomedical
Materials Science, Biomaterials
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