Redox-Enabled Pathway Complexity in Supramolecular Hydrogels

Pathway complexity in supramolecular assemblies presents a unique opportunity for a single, relatively simple system to exhibit a wide range of properties, allowing for multifunctionality. In this study, we report redox-enabled pathway complexity in amino acid-functionalized perylene diimides (PDIs) and its consequence for the macroscopic hydrogel network. We show that chemical reduction and subsequent oxidation enable a kinetically trapped state of the micellar network, which transforms into different network morphologies in response to heat and time. Our finding that pathway complexity in supramolecular systems can alter bulk material properties suggests the potential for future development of dynamic materials that achieve multiple macroscopic functions with a single building block.