High-Performance Flexible Solid-State Carbon Cloth Supercapacitors Based on Highly Processible N-Graphene Doped Polyacrylic Acid/Polyaniline Composites

Improving the solubility of conductive polymers to facilitate processing usually decreases their conductivity and they suffer from poor cycling stability due to swelling-shrinking during charging cycles. We circumvent these problems with a novel preparation method for nitrogen-doped graphene (NG) enhanced polyacrylic acid/polyaniline (NG-PAA/PANI) composites, ensuring excellent processibility for scalable production. The content of PANI is maximized under the constraint of still allowing defect-free coatings on filaments of carbon cloth (CC). The NG content is then adjusted to optimize specific capacitance. The optimal CC electrodes have 32 wt.% PANI and 1.3 wt.% NG, thus achieving a high capacitance of 521 F/g at 0.5 F/g. A symmetric supercapacitor made from 20 wt.% PANI CC electrodes has more than four times the capacitance (68 F/g at 1 A/g) of previously reported flexible capacitors based on PANI-carbon nanotube composites and it retains the full capacitance under large bending angles. The capacitor exhibits high energy and power densities (5.8 Wh/kg at 1.1 kW/kg), a superior rate capability (still 81% of the 1 A/g capacitance at 10 A/g) and long-term electrochemical stability (83.2% retention after 2000 cycles).