3D-Printable, Self-Stiffening (4D) and Shape Morphing Hydrogel through Single-Step Orthogonal Crosslinking of Phenolic Biopolymers for Dynamic Tissue Engineering

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dc.authorid0000-0002-6490-0329
dc.authorid0000-0001-5558-0995
dc.authorid0000-0003-3445-1814
dc.contributor.authorGungor, Nuriye Nazet
dc.contributor.authorKurt, Tugce
dc.contributor.authorSari, Buse
dc.contributor.authorIsik, Melis
dc.contributor.authorOkesola, Babatunde O.
dc.contributor.authorArslan, Yavuz Emre
dc.contributor.authorDerkus, Burak
dc.date.accessioned2026-02-03T12:03:19Z
dc.date.available2026-02-03T12:03:19Z
dc.date.issued2025
dc.departmentÇanakkale Onsekiz Mart Üniversitesi
dc.description.abstractParticularly for dynamic, shape-changing, or fibrillar tissues such as muscles and blood vessels, the development of innovative biomaterials is crucial for advancing tissue engineering and regenerative medicine. This study introduces a novel multicomponent hydrogel created from silk fibroin (SF), tyramine-modified hyaluronic acid (HA_Tyr), and tyramine-modified gelatin (G_Tyr). Using an enzymatic orthogonal covalent bonding between phenolic groups, i.e., tyrosine and tyramine moieties of SF, HA_Tyr, and G_Tyr, a dynamically stiffening SF/HA_Tyr/G_Tyr (SHG) multicomponent hydrogel is achieved with enhanced mechanical properties. Utilizing an extrusion-based 3D printing approach, the precise fabrication of constructs with tailored geometries and functionalities is demonstrated. The emerging 3D-printed hydrogels undergo morphologic changes (4D) under 37 degrees C/phosphate buffer saline (PBS) conditions. The observed morphological change results from the conformational change and folding of SF leading to fibrillation. These multicomponent hydrogels also show significant promise in creating bio-instructive materials that meet the mechanical and functional requirements necessary for in situ tissue engineering. The study highlights the potential of these self-stiffening biomaterials to recover dynamic and fibrillar tissues, supported by both in vitro and pre-clinical chorioallantoic membrane (CAM) model evaluations that underscore their biocompatibility and pro-angiogenic properties.
dc.description.sponsorshipHealth Institute of Turkey (TUSEB) [22617]
dc.description.sponsorshipTurkish Academy of Science (TUBA)
dc.description.sponsorshipScience Academy (Istanbul)
dc.description.sponsorshipUniversity of Nottingham for the Award of Nottingham Research Fellowship
dc.description.sponsorshipN.N.G. and T.K. contributed equally to this work. The authors B.D. and Y.E.A. express gratitude to the Health Institute of Turkey (TUSEB) for funding this project (Grant No: 22617). B.D. also acknowledges the Turkish Academy of Science (TUBA) and the Science Academy (Istanbul) for their support. B.O.O. acknowledged the University of Nottingham for the Award of Nottingham Research Fellowship
dc.identifier.doi10.1002/adhm.202501733
dc.identifier.issn2192-2640
dc.identifier.issn2192-2659
dc.identifier.pmid40832767
dc.identifier.scopus2-s2.0-105013753615
dc.identifier.scopusqualityQ1
dc.identifier.urihttps://doi.org/10.1002/adhm.202501733
dc.identifier.urihttps://hdl.handle.net/20.500.12428/35025
dc.identifier.wosWOS:001553683800001
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoen
dc.publisherWiley
dc.relation.ispartofAdvanced Healthcare Materials
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_WOS_20260130
dc.subject3D printing
dc.subjectdynamic tissue engineering
dc.subjectphenolic biopolymers
dc.subjectself-stiffening hydrogel
dc.title3D-Printable, Self-Stiffening (4D) and Shape Morphing Hydrogel through Single-Step Orthogonal Crosslinking of Phenolic Biopolymers for Dynamic Tissue Engineering
dc.typeArticle

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