Modulating Supramolecular Peptide Hydrogel Viscoelasticity Using Biomolecular Recognition

• Published in: Biomacromolecules 2017-11, Vol.18 (11), p.3591-3599
• Main Authors: DiMaio, John T. M, Doran, Todd M, Ryan, Derek M, Raymond, Danielle M, Nilsson, Bradley L
• Format: Article
• Language: English
• Subjects: Biocompatible Materials - chemical synthesis; Biocompatible Materials - chemistry; Drug Delivery Systems; Elasticity; Humans; Hydrogel, Polyethylene Glycol Dimethacrylate - chemical synthesis; Hydrogel, Polyethylene Glycol Dimethacrylate - chemistry; Peptide Nucleic Acids - chemical synthesis; Peptide Nucleic Acids - chemistry; Peptides - chemical synthesis; Peptides - chemistry; Polymers - chemical synthesis; Polymers - chemistry; Tissue Engineering
• ISSN: 1525-7797; 1526-4602
• DOI: 10.1021/acs.biomac.7b00925

Self-assembled peptide-based hydrogels are emerging materials that have been exploited for wound healing, drug delivery, tissue engineering, and other applications. In comparison to synthetic polymer hydrogels, supramolecular peptide-based gels have advantages in biocompatibility, biodegradability, and ease of synthesis and modification. Modification of the emergent viscoelasticity of peptide hydrogels in a stimulus responsive fashion is a longstanding goal in the development of next-generation materials. In an effort to selectively modulate hydrogel viscoelasticity, we report herein a method to enhance the elasticity of β-sheet peptide hydrogels using specific molecular recognition events between functionalized hydrogel fibrils and biomolecules. Two distinct biomolecular recognition strategies are demonstrated: oligonucleotide Watson–Crick duplex formation between peptide nucleic acid (PNA) modified fibrils with a bridging oligonucleotide and protein–ligand recognition between mannose modified fibrils with concanavalin A. These methods to modulate hydrogel elasticity should be broadly adaptable in the context of these materials to a wide variety of molecular recognition partners.