Sustainable Energy Storage Systems: Polypyrrole-Filled Polyimide-Modified Carbon Nanotube Sheets with Remarkable Energy Density

Organic hybrid materials are gaining traction as electrode candidates for energy storage due to their structural tunability and environmental compatibility. This study investigates polyimide/carbon nanotube/polypyrrole (PI/CNTs/PPy) hybrid nanocomposites, focusing on the correlation between thermal imidization temperature, polypyrrole deposition time, and the resulting electrochemical properties. By modulating PI processing temperatures (90 °C, 180 °C, 250 °C) and PPy deposition durations (60–700 s), this research uncovers critical structure–function relationships governing charge storage behavior. Scanning electron microscopy and electrochemical impedance spectroscopy reveal that low-temperature imidization preserves porosity and enables ion-accessible pathways, while moderate PPy deposition enhances electrical conductivity without blocking pore networks. The optimized composite, processed at 90 °C with 60 s PPy deposition, demonstrates superior specific capacitance (850 F/g), high redox contribution (~70% of total charge), low charge transfer resistance, and enhanced energy/power density. In contrast, high-temperature processing and prolonged PPy deposition result in structural densification, increased resistance, and diminished performance. These findings highlight a synergistic design approach that leverages partial imidization and controlled doping to balance ionic diffusion, electron transport, and redox activity. The results provide a framework for developing scalable, high-performance, and sustainable electrode materials for next-generation lithium-ion batteries and supercapacitors.