Electrochemical Switching of Laser-Induced Graphene/Polymer Composites for Tunable Electronics

Laser reduction of graphene oxide (GO) is a promising approach for achieving flexible, robust, and electrically conductive graphene/polymer composites. Resulting composite materials show significant technological potential for energy storage, sensing, and bioelectronics. However, in the case of insulating polymers, the properties of electrodes show severely limited performance. To overcome these challenges, we report on a post-processing redox treatment that allows the tuning of the electrochemical properties of laser-induced rGO/polymer composite electrodes. We show that the polymer substrate plays a crucial role in the electrochemical modulation of the composites' properties, such as the electrode impedance, charge transfer resistance, and areal capacitance. The mechanism behind the reversible control of electrochemical properties of the rGO/polymer composites is the cleavage of polymer chains in the vicinity of rGO flakes during redox cycling, which exposes rGO active sites to interact with the electrolyte. Sequential redox cycling improves composite performance, allowing the development of devices such as electrolyte-gated transistors, which are widely used in chemical sensing applications. Our strategy enables the engineering of the electrochemical properties of rGO/polymer composites by post-treatment with dynamic switching, opening up new possibilities for flexible electronics and electrochemical applications having tunable properties.