Cartilage-like protein hydrogels engineered via entanglement

Linglan Fu, Lan Li, Qingyuan Bian, Bin Xue, Jing Jin, Jiayu Li, Yi Cao, Qing Jiang and Hongbin Li ()
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Linglan Fu: The University of British Columbia
Lan Li: Drum Tower Hospital affiliated to Medical School of Nanjing University
Qingyuan Bian: The University of British Columbia
Bin Xue: Nanjing University
Jing Jin: Drum Tower Hospital affiliated to Medical School of Nanjing University
Jiayu Li: The University of British Columbia
Yi Cao: Nanjing University
Qing Jiang: Drum Tower Hospital affiliated to Medical School of Nanjing University
Hongbin Li: The University of British Columbia

Nature, 2023, vol. 618, issue 7966, 740-747

Abstract: Abstract Load-bearing tissues, such as muscle and cartilage, exhibit high elasticity, high toughness and fast recovery, but have different stiffness (with cartilage being significantly stiffer than muscle)1–8. Muscle achieves its toughness through finely controlled forced domain unfolding–refolding in the muscle protein titin, whereas articular cartilage achieves its high stiffness and toughness through an entangled network comprising collagen and proteoglycans. Advancements in protein mechanics and engineering have made it possible to engineer titin-mimetic elastomeric proteins and soft protein biomaterials thereof to mimic the passive elasticity of muscle9–11. However, it is more challenging to engineer highly stiff and tough protein biomaterials to mimic stiff tissues such as cartilage, or develop stiff synthetic matrices for cartilage stem and progenitor cell differentiation12. Here we report the use of chain entanglements to significantly stiffen protein-based hydrogels without compromising their toughness. By introducing chain entanglements13 into the hydrogel network made of folded elastomeric proteins, we are able to engineer highly stiff and tough protein hydrogels, which seamlessly combine mutually incompatible mechanical properties, including high stiffness, high toughness, fast recovery and ultrahigh compressive strength, effectively converting soft protein biomaterials into stiff and tough materials exhibiting mechanical properties close to those of cartilage. Our study provides a general route towards engineering protein-based, stiff and tough biomaterials, which will find applications in biomedical engineering, such as osteochondral defect repair, and material sciences and engineering.

Date: 2023
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DOI: 10.1038/s41586-023-06037-0

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