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Tuning the life-time of supramolecular hydrogels using ROS-responsive telechelic peptide-polymer conjugates

R. Otter,Christian M. Berač,S. Seiffert,Pol Besenius

Published 2019 in European Polymer Journal

ABSTRACT

Abstract The synthesis of multi-stimuli responsive peptide-poly(ethylene glycol) ABA-type conjugates is reported. The β-sheet encoded intramolecular folding and intermolecular self-assembly into 1D nanorods is based on a phenylalanine(F)-methionine(M)-histidine(H) FMHMHF hexapeptide sequence, and the supramolecular nanorods are stabilised by a shielding corona of hydrophilic PEG polymers. Interstrand crosslinking leads to the formation of physical networks and hydrogels at physiological pH and at room temperature. The thioether functional groups integrate oxidation responsive properties in the supramolecular polymer assemblies. We show that the glucose fuelled and glucose oxidase catalysed production of the reactive oxygen species (ROS) leads to transiently stable supramolecular hydrogels that operate in a fully autonomous reaction set-up, with a tuneable gelation life-times of 1–12 h. ROS play an important role in signalling cascades and inflammation processes. We are therefore particularly interested in further developing our strategy for the design of biomaterials for applications in redox microenvironments.

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