Chen, Shiyi, Hassan, Nourhan ORCID: 0000-0003-3189-8063, Kopp, Alexander, Eufrásio-da-Silva, Tatiane, Arfaoui, Jihene ORCID: 0000-0003-2158-1185, Isella, Benedetta, Aytuna, Ziyaad, Barnowski, Philipp, Sengle, Gerhard, Dolatshahi-Pirouz, Alireza, Kröger, Nadja and Maleki, Hajar Homa ORCID: 0000-0002-2813-4700 (2025). Theragenerative injectable bone-adhesive hydrogels for combined photothermal osteosarcoma therapy and bone repair. Biomaterials Science, 13 (13). pp. 3544-3560. Royal Society of Chemistry. ISSN 2047-4830

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Identification Number:10.1039/D5BM00559K

Abstract

Injectable hydrogels with self-healing properties, tissue adhesion, biocompatibility, and cancer therapeutic capabilities offer a promising solution for addressing bone loss and residual tumor cells following surgical resection of osteosarcoma. In this study, injectable adhesive hybrid hydrogels were developed using natural silk-derived proteins, silk fibroin (SF), and silk sericin (SS). The sericin was surface functionalized with dopamine (DOPA) forming SSDOPA, while the silk fibroin was enzymatically oxidized (forming SFO) to introduce abundant catechol moieties on the polymer chains. These modifications enabled hydrogelation and self-assembly in the presence of copper ions (Cu 2+ ) and tannic acid (TA), creating an SFO-SSDopa-Cu 2+ -TA hydrogel inspired by the mussel adhesion mechanism. The dynamic metal-catechol coordination bonds, along with other covalent and non-covalent interactions in the gel network, imparted excellent shear-thinning properties with 3D printability, injectability, self-healing (72.27 ± 9.35% after 6 cyclic), making it suitable for minimally invasive surgeries and targeted delivery applications. Additionally, the developed adhesive hydrogel demonstrated strong adhesiveness (664.03 ± 15.87 kPa and 854.15 ± 12.90 kPa on Gel- and Hap-based substrates respectively), showing excellent bonding performance to natural bone and tissue. Its black coloration enabled efficient absorption of near-infrared (NIR) light (reach 45–48 °C), facilitating the eradication of almost 60% osteosarcoma cells through photothermal therapy within 20 minutes of hydrogel irradiation with laser. Moreover, the developed SFO-SSDopa-Cu 2+ -TA hydrogels promoted the proliferation and migration of pre-osteoblast cells, confirming their excellent biocompatibility. Coupled with good biodegradability, these hydrogels demonstrate significant potential as theragenerative materials for minimally invasive osteosarcoma treatment, providing a clinically translatable solution for repairing bone affected by the disease.

Item Type: Article
Creators:
Creators
Email
ORCID
ORCID Put Code
Chen, Shiyi
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Hassan, Nourhan
UNSPECIFIED
UNSPECIFIED
Kopp, Alexander
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Eufrásio-da-Silva, Tatiane
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Arfaoui, Jihene
UNSPECIFIED
UNSPECIFIED
Isella, Benedetta
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Aytuna, Ziyaad
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Barnowski, Philipp
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Sengle, Gerhard
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Dolatshahi-Pirouz, Alireza
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Kröger, Nadja
UNSPECIFIED
UNSPECIFIED
UNSPECIFIED
Maleki, Hajar Homa
UNSPECIFIED
UNSPECIFIED
URN: urn:nbn:de:hbz:38-811671
Identification Number: 10.1039/D5BM00559K
Journal or Publication Title: Biomaterials Science
Volume: 13
Number: 13
Page Range: pp. 3544-3560
Number of Pages: 17
Date: 2025
Publisher: Royal Society of Chemistry
ISSN: 2047-4830
Language: English
Faculty: Faculty of Mathematics and Natural Sciences
Faculty of Medicine
Divisions: CECAD - Cluster of Excellence Cellular Stress Responses in Aging-Associated Diseases
Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Inorganic Chemistry
Faculty of Medicine > Biochemie > Zentrum für Biochemie
Faculty of Medicine > Kinder- und Jugendmedizin > Klinik und Poliklinik für Kinder- und Jugendmedizin
Zentrum für Molekulare Medizin
Subjects: Medical sciences Medicine
['eprint_fieldname_oa_funders' not defined]: Publikationsfonds UzK
Refereed: Yes
URI: http://kups.ub.uni-koeln.de/id/eprint/81167

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