Modulating Supramolecular Peptide Hydrogel Viscoelasticity Using Biomolecular Recognition

Biomacromolecules. 2017 Nov 13;18(11):3591-3599. doi: 10.1021/acs.biomac.7b00925. Epub 2017 Sep 14.


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.

MeSH terms

  • 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


  • Biocompatible Materials
  • Peptide Nucleic Acids
  • Peptides
  • Polymers
  • Hydrogel, Polyethylene Glycol Dimethacrylate