Redox-Mediated, Transient Supramolecular Charge-Transfer Gel and Ink

Unprecedented spatiotemporal control exhibited by natural systems has aroused interest in the construction of its synthetic mimics. Cytoskeleton proteins utilize fuel-driven dissipative self-assembly to temporally regulate cell shape and motility. Until now, synthetic efforts have majorly contributed to fundamental strategies; however, temporally programmed functions are rarely explored. Herein, we work toward alleviating this scenario by using a charge-transfer (CT) based supramolecular polymer that undergoes structural changes under the effect of a redox fuel. The structural changes in supramolecular assembly amplify into observable macroscopic and material property changes. As a result, we achieve transient chemochromism, a self-erasing ink and self-regenerating hydrogel, whose temporal profile can be regulated by varying the concentrations of the chemical cues (fuel and enzyme). The redox-mediated transient functions in the CT based supramolecular polymer pave way to create next-generation active, adaptive, and autonomous smart materials.