A supercapacitor is an electrical energy storage system with high power output. With worldwide awareness of sustainable development, developing cost-effective, environmentally friendly, and high-performance supercapacitors is an important research direction. The use of sustainable components like wood biochar in the electrode materials for supercapacitor uses holds great promise for sustainable supercapacitor development. In this study, we demonstrated a facile and powerful approach to prepare meso-microporous carbon electrode materials for sustainable and high-performance supercapacitor development by electrospinning polyacrylonitrile (PAN) with F-treated biochar and subsequent aerogel construction followed by stabilization, carbonization, and carbon activation. The resultant carbon nanofibrous aerogel electrode material (ENFA-FBa) exhibited exceptional specific capacitance, attributing to enormously increased micropore and mesopore volumes, much more activated sites to charge storage, and significantly greater electrochemical interaction with electrolyte. This electrode material achieved a specific capacitance of 407 F/g at current density of 0.5 A/g in 1 M H₂SO₄ electrolyte, which outperformed the state-of-the-art specific capacitance of biochar-containing electrospun carbon nanofibrous aerogel electrode materials (<300 F/g). A symmetric two-electrode cell with ENFA-FBa as electrode material showed an energy density of 11.2 Wh/kg at 125 W/kg power density. Even after 10,000 cycles of charging-discharging at current density of 10 A/g, the device maintained a consistent coulombic efficiency of 53.5% and an outstanding capacitance retention of 91%. Our research pointed out a promising direction to develop sustainable electrode materials for future high-performance supercapacitors.

Carbon nanofibrous materials from electrospinning are good candidate electrode materials for supercapacitor applications due to their straightforward processability, chemical stability, high porosity, and large surface area. In this research, a straightforward and effective way was revealed to significantly enhance the electrochemical performance of carbon nanofibrous electrode material from electrospinning of polyacrylonitrile (PAN). Fluorination of the electrospun carbon nanofibers (ECNF) was studied by comparing two types of hydrofluoric acid (HF) treatment, i.e., direct HF acid treatment on ECNF (Type I) vs. HF acid treatment on the stabilized PAN (Type II) followed by carbonization. The latter was found to be an advantageous way to introduce C-F bonds in the resultant carbon nanofibrous electrode material that contributed to pseudocapacitance. Furthermore, the Type II HF acid treatment demonstrated exciting synergistic effects with ECNF aerogel formation on carbon structure and porosity development and generated a superior fluorinated electrospun carbon nanofibrous aerogel (ECNA-F) electrode material for supercapacitor uses. The resultant ECNA-F electrode material demonstrated excellent electrochemical performance with great cyclic stability due to the large improvements in both pseudocapacitance and electrical double-layer capacitance. ECNA-F achieved a specific capacitance of 372 F/g at a current density of 0.5 A/g with 1 M H₂SO₄ electrolyte, and the device with ECNA-F and 1 M Na₂SO₄ electrolyte possessed an energy density of 29.1 Wh/kg at a power density of 275 W/kg. This study provided insight into developing high-performance and stable carbon nanofibrous electrode materials for supercapacitors.