Single-Step Electrochemical Synthesis of PEDOT-NG Nanoarchitecture via Multifunctional Electrolytes for High-Performance Pseudocapacitors

The development of high-performance pseudocapacitors based on conducting polymers has been severely constrained by fundamental challenges, including poor cycling stability, limited ionic accessibility, and complex multistep synthesis procedures. Here, we demonstrate a revolutionary one-pot electrodeposition approach utilizing lithium nanographenide (LNG) as a multifunctional electrolyte that simultaneously serves as supporting electrolyte, anionic dopant, and structural modifier for the electrochemical synthesis of the poly(3,4-ethylenedioxythiophene) (PEDOT) nanoarchitecture. Unlike conventional approaches requiring postsynthesis doping or complex composite fabrication, our method enables direct formation of the optimized PEDOT-nanographenide (PEDOT-NG) nanoarchitecture through a single electrochemical step. The nanographenide polyanions (NGn-) facilitate real-time polymer backbone modification through π-π stacking interactions and electrostatic doping, transitioning PEDOT from benzenoid to quinoidal structures while creating interconnected three-dimensional porous networks. The resulting PEDOT-NG nanoarchitecture achieves an exceptional specific capacitance of 259 F g⁻¹ at 1.0 A g⁻¹ with an outstanding cycling stability of 80.2% retention after 5,000 cycles in aqueous electrolyte─representing a significant advancement beyond current state-of-the-art PEDOT-based pseudocapacitors. This multifunctional electrolyte strategy represents a paradigm shift in pseudocapacitor electrode design, offering a scalable pathway toward high-performance energy storage devices with potential applications in electric vehicles and grid-scale energy storage.