Tunable Pentapeptide Self‐Assembled β‐Sheet Hydrogels

Abstract

Oligopeptide‐based supramolecular hydrogels hold promise in a range of applications. The gelation of these systems is hard to control, with minor alterations in the peptide sequence significantly influencing the self‐assembly process. We explored three pentapeptide sequences with different charge distributions and discovered that they formed robust, pH‐responsive hydrogels. By altering the concentration and charge distribution of the peptide sequence, the stiffness of the hydrogels could be tuned across two orders of magnitude (2–200 kPa). Also, through reassembly of the β‐sheet interactions the hydrogels could self‐heal and they demonstrated shear‐thin behavior. Using spectroscopic and cryo‐imaging techniques, we investigated the relationship between peptide sequence and molecular structure, and how these influence the mechanical properties of the hydrogel. These pentapeptide hydrogels with tunable morphology and mechanical properties have promise in tissue engineering, injectable delivery vectors, and 3D printing applications.

Design Principles for Aqueous Interactive Materials: Lessons from Small Molecules and Stimuli‐Responsive Systems

“…A simple and robust pH‐responsive hydrogel was produced by Scherman and co‐workers, who reported the production of hydrogels formed from three pentapeptide sequences based on the amino acids Isoleucine (I) and Aspartate (D): IDIDI DDIII and DIID 96. Upon addition of HCl, the concentration and charge distribution of the peptide sequence was altered.…”

Preparation and applications of peptide-based injectable hydrogels

“…Scherman et al explored and screened a pentapeptide hydrogel (IDIDI) with tunable morphology and mechanical properties produced through reassembly of the b-sheet interactions, which showed potential applications in delivery systems and tissue engineering. 29 The primary effect of physically cross-linked hydrogels is the formation of physical crosslinking points inside the gels. In 1993, Zhang et al 30 reported that a 16-residue peptide [(Ala-Glu-Ala-Glu-Ala-Lys-Ala-Lys) 2 ] (EAK16) could spontaneously assemble into a hydrogel structure in the presence of salt, which opened up the new eld of self-assembly technology of polypeptide molecules.…”

Royal Society of Chemistry Prizes and Awards 2018

“…Scherman's research focuses on dynamic supramolecular self‐assembly at interfaces though the application of macrocyclic host–guest chemistry. He has reported in Angewandte Chemie on pentapeptide self‐assembled β‐sheet hydrogels …”