Abstract
Spatial and temporal control in multi-stimuli-responsive materials are critical properties to advance and optimize functional soft matter in order to mimic key features of living systems. In this contribution, I will discuss our methodology in developing non-equilibrium states in supramolecular materials. We have expanded our concept of charge regulated s–sheet self-assembly of alternating hydrophilic and hydrophobic amino acids in order to introduce redox-switchable properties. An interplay of pH- and oxidation-stimuli, promoted by the production of reactive oxygen species (ROS) thus leads to transient supramolecular polymerizations of methionine containing amphiphiles, with tuneable lifetimes and stabilities of the hydrogels. The incorporation of triethylene glycol chains introduces thermoresponsive properties to the materials, which operates in a biomedically relevant temperature range of 30 - 40 °C. Excitingly repair enzymes are able to reverse the oxidative damage in the methionine-based thioether side chains. Since reactive oxygen species play an important role in signal transduction cascades, our materials offer great potential for applications of these dynamic biomaterials in redox microenvironments.
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