Natural N/O/S co-doped defect-rich functional carbon materials for aqueous supercapacitors: Effect mechanism of N-containing functional groups on chemical activation

Abstract

The efficient synthesis of porous carbons with a micro-mesoporous composite structure from low-cost, multi-source biomass was of significant importance for the fabrication of carbon-based supercapacitors. A novel method for the preparation of micro-mesoporous composite carbon materials by co-pyrolysis of multi-source biomass coupled with KOH activation was proposed in this study. The N, O and S co-doped micro-mesoporous composite carbon materials were synthesized using the bamboo and spiral algae as the precursors and KOH as the activator. Spiral algae, as the main source of heteroatoms, played multiple roles (pore forming agent, dopant and enhancer) in the co-pyrolysis process. The enhanced effect of heteroatom doping on KOH activation facilitated the formation of microporous structures. The KCA-500–2 exhibited a porous structure dominated by micropores, with a specific surface area (SSA) of 2421.85 m2/g. At 0.5 A/g, KCA-500–2 displayed an excellent capacitance of 460F/g and outstanding rate performance (73.5 %). The assembled aqueous symmetric supercapacitor (KCA//KCA) demonstrated a maximum energy density of 19.09 Wh/kg at a power density of 150 W/kg. In addition, KCA//KCA attained 97.96 % capacitance retention after 9,000 cycles. This work revealed the synergistic mechanism between N-containing functional groups and KOH activation, suggesting a theoretical guidance for the synthesis of high-performance supercapacitors.