Bioinspired Out-of-Equilibrium Conductive Hydrogels: Unlocking Fuel and Light-Responsive Transient Conducting Properties

The development of out-of-equilibrium supramolecular hydrogels, inspired by biological systems, has attracted considerable interest due to their potential applications in nanotechnology. Despite this, these transient hydrogels' (opto-)electronic properties remain elusive. This study introduces a bioinspired dissipative hydrogel powered by a chemical fuel, exhibiting tunable conducting and photoelectronic functionalities. A bio-organic bolaamphiphile (PA) was designed and synthesized, integrating the optoelectronic characteristics of perylene diimide (P) with the reversible gel-triggered switching capabilities of l-aspartic acid (A). Precise temporal control over the supramolecular self-assembly and disassembly of the PA hydrogel was achieved by regulating the chemical fuel dimethyl sulfate (DMS). Results demonstrate that the PA-based dissipative self-assembly can reversibly switch between an insulating sol state and a conductive gel state, accompanied by nanostructural, fluorescence, and chiroptical switching. Furthermore, a thin film derived from the hydrogel exhibited photoresponsive conductivity switching capability. PA's transient structural, chemical, and functional properties were extensively characterized using spectroscopic, microscopic, computational, and device fabrication techniques. This study not only elucidates the structure-property relationships in dissipative hydrogels but also contributes to the development of adaptive, life-like functional nanomaterials with promising applications in optoelectronics, nanotechnology, and soft robotics.