Nacre-inspired, strong, tough silk fibroin hydrogels based on biomineralization and the layer-by-layer assembly of ordered silk fabric

• Published in: International journal of biological macromolecules Vol. 253; p. 126730
• Main Authors: Zong, Chen-Man, Shuang, Fei-Fan, Chen, Jie, Wang, Ping-Yue, Li, Jing-Rou, Zhang, Dong-Yang, Song, Peng, Chen, Tao, Zhao, Wei-Guo, Yao, Xiao-Hui
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 31.12.2023
• Subjects: Hydrogel; Multidimensional design; Silk fibroin; Structural materials; Silk fibroin; Structural materials; Hydrogel; Multidimensional design
• ISSN: 0141-8130; 1879-0003
• DOI: 10.1016/j.ijbiomac.2023.126730

Hydrogels are attractive materials with structures and functional properties similar to biological tissues and widely used in biomedical engineering. However, traditional synthetic hydrogels possess poor mechanical strength, and their applications are limited. Herein, a multidimensional material design method is developed; it includes the in situ gelation of silk fabric and nacre-inspired layer-by-layer assembly, which is used to prepare silk fibroin (SF) hydrogels. The in situ gelation method of silk fabric introduces a directionally ordered fabric network in a silk substrate, considerably enhancing the strength of hydrogels. Based on the nacre structure, the layer-by-layer assembly method enables silk hydrogels to break through the size limit and increase the thickness, realizing the longitudinal extension of the hydrogels. The application of the combined biomineralization and hot pressing method can effectively reduce interface defects and improve the interaction between organic and inorganic interfaces. The multidimensional material design method helps increase the strength (287.78 MPa), toughness (18.43 MJ m−3), and fracture energy (50.58 kJ m−2) of SF hydrogels; these hydrogels can weigh 2000 times their own weight. Therefore, SF hydrogels designed using the aforementioned combined method can realize the combination of strength and toughness and be used in biological tissue engineering and structural materials. •In situ gelation method successfully introduced ordered silk fabric network.•Nacre-inspired structure was constructed by layer-by-layer assembly method.•The combination of biomineralization and hot pressing reduced interface defects.•This silk fibroin hydrogel realized the combination of high strength and toughness.