PEDOT:PSS-Induced Supramolecular G-Quartet Hydrogel for Diffusion-Controlled High-Performance Flexible Supercapacitor

Soft and wearable electronics require conductive hydrogels that combine efficient charge storage with biocompatibility and structural adaptability. Herein, we demonstrate PEDOT:PSS as a structure-directing agent that induces self-assembly of the biomolecule 5′-GMP into a fibrillar network, forming a supramolecular conductive hydrogel. Cooperative hydrogen bonding and electrostatic interactions between the sulfonate groups of PSS and the phosphate groups of GMP drive hierarchical G-quadruplex assembly, producing an injectable and printable hydrogel with tissue-like softness. Although pristine PEDOT:PSS dispersions show limited charge-storage capability, this performance is greatly enhanced in the hydrogel architecture. The GMP fibrillar network encapsulating PEDOT:PSS creates continuous Na+-ion diffusion channels, enabling efficient ion transport and diffusion-controlled pseudocapacitive storage. As a flexible electrode, the hydrogel enables an all-solid-state symmetric supercapacitor delivering a specific capacitance of 1436 F g–1 of a single electrode and an energy density of 71.8 Wh kg–1 with excellent cycling stability and mechanical flexibility.