Bioinspired Reversibly Cross‐linked Hydrogels Comprising Polypeptide Micelles Exhibit Enhanced Mechanical Properties |
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Authors: | Ali Ghoorchian Joseph R Simon Bhuvnesh Bharti Wei Han Xuanhe Zhao Ashutosh Chilkoti Gabriel P López |
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Affiliation: | 1. NSF Research Triangle Materials Research Science and Engineering Center, Department of Biomedical Engineering, Duke University, Durham, NC, USA;2. NSF Research Triangle Materials Research Science and Engineering Center, Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC, USA;3. Soft Active Materials Laboratory, Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA;4. NSF Research Triangle Materials Research Science and Engineering Center, Department of Mechanical Engineering and Materials Science, Duke University, Durham, NC, USA |
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Abstract: | Noncovalently cross‐linked networks are attractive hydrogel platforms because of their facile fabrication, dynamic behavior, and biocompatibility. The majority of noncovalently cross‐linked hydrogels, however, exhibits poor mechanical properties, which significantly limit their utility in load bearing applications. To address this limitation, hydrogels are presented composed of micelles created from genetically engineered, amphiphilic, elastin‐like polypeptides that contain a relatively large hydrophobic block and a hydrophilic terminus that can be cross‐linked through metal ion coordination. To create the hydrogels, heat is firstly used to trigger the self‐assembly of the polypeptides into monodisperse micelles that display transition metal coordination motifs on their coronae, and subsequently cross‐link the micelles by adding zinc ions. These hydrogels exhibit hierarchical structure, are stable over a large temperature range, and exhibit tunable stiffness, self‐healing, and fatigue resistance. Gels with polypeptide concentration of 10%, w/v, and higher show storage moduli of ≈1 MPa from frequency sweep tests and exhibit self‐healing within minutes. These reversibly cross‐linked, hierarchical hydrogels with enhanced mechanical properties have potential utility in a variety of biomedical applications. |
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Keywords: | bioinspired materials hydrogels micelles elastin‐like polypeptides self‐healing |
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