Solid-State Precursor Impregnation for Enhanced Capacitance in Hierarchical Flexible Poly(3,4-Ethylenedioxythiophene) Supercapacitors

Increasing capacitance and energy density is a major challenge in developing supercapacitors for flexible portable electronics. A thick electrode with a high mass loading of active electronic material leads to high areal capacitance; however, the higher the loading, the higher the mechanical stiffness and ion diffusion resistance, thereby hampering development of flexible supercapacitors. Here, we show a chemical strategy that leads to a hierarchical electrode structure producing devices with both an exceedingly high areal capacitance and superior flexibility. We utilize α-Fe2O3 particles as an oxidant precursor for controlling oxidative radical polymerization of the conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) from the vapor phase. Our approach impregnates carbon cloth with α-Fe2O3 particles prior to monomer vapor exposure, resulting in state-of-the-art flexible nanofibrillar PEDOT supercapacitors possessing high areal capacitance (2243 mF/cm2 for two-electrode vs 6210 mF/cm2 for three-electrode) and high areal energy density (412 μWh/cm2).