Polypeptide-based self-healing hydrogels: Design and biomedical applications

Self-healing hydrogels can heal themselves on the damaged sites, which opens up a fascinating way for enhancing lifetimes of materials. Polypeptide/poly(amino acid) is a class of polymers in which natural amino acid monomers or derivatives are linked by amide bonds with a stable and similar secondary structure as natural proteins (alpha-helix or beta-fold). They have the advantages of nontoxicity, biodegradability, and low immunogenicity as well as easy modification. All these properties make polypeptides extremely suitable for the preparation of self-healing hydrogels for biomedical applications. In this review, we mainly focus on the progress in the fabrication strategies of polypeptide-based self-healing hydrogels and their biomedical applications in the recent 5 years. Various crosslinking methods for the preparation of polypeptide-based self-healing hydrogels are first introduced, including host-guest interactions, hydrogen bonding, electrostatic interactions, supramolecular self-assembly of beta-sheets, and reversible covalent bonds of imine and hydrazone as well as molecular multi-interactions. Some representative biomedical applications of these self-healing hydrogels such as delivery system, tissue engineering, 3D-bioprinting, antibacterial and wound healing as well as bioadhesion and hemostasis are also summarized. Current challenges and perspectives in future for these "smart" hydrogels are proposed at the end. Statement of Significance Polypeptides with the advantages of nontoxicity, biodegradability, hydrophilicity and low immunogenicity, are extremely suitable for the preparation of self-healing hydrogels in biomedical applications. Recently, the researches of polypeptide-based self-healing hydrogel have drawn the great attentions for scientists and engineers. A review to summarize the recent progress in design and biomedical applications of these polypeptide-based self-healing hydrogels is highly needed. In this review, we mainly focus on the progress in fabrication strategies of polypeptide-based self-healing hydrogels and biomedical applications in recent five years and aim to draw the increased attention to the importance of these "smart" hydrogels, facilitating the advances in biomedical applications. We believe this work would draw interest from readers of Acta Biomaterialia. (C) 2020 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.