Conjugated polymer-based carbonaceous films as binder-free carbon electrodes in supercapacitors

We present a facile preparation method for carbonaceous film electrodes using poly(3,4-ethylenedioxythiophene) (PEDOT) and polyacetylene (PA) films as precursors via a morphology-retaining carbonization process. Carbonization was performed on acceptor-doped conjugated polymer films in the temperature range of 600-1100 °C. The obtained carbonaceous films had similar surface morphologies to those of the original conjugated polymer films. The carbonaceous film prepared from the electrochemically synthesized PEDOT film and the carbon film prepared from the chemically synthesized PA film showed hierarchical porous structures consisting of granular and fibril morphologies, respectively. The PEDOT and PA films carbonized at 1100 °C exhibited average electrical conductivities of 2.1 × 10⁰ S cm^-1 and 9.9 × 10¹ S cm^-1, respectively. The carbonaceous films could be used as binder-free carbon electrodes in supercapacitors, and the PEDOT-based carbonaceous film prepared in the range of 1000-1100 °C exhibited the most efficient performance on the basis of the electrochemical capacitance in neutral and alkaline aqueous solutions determined from cyclic voltammograms and galvanostatic charge/discharge curves. This approach requires no binders/additives and no further activation processes or additional treatments for the enhancement of the capacities of the carbon materials, enabling one-step fabrication and their direct use as carbon electrodes for energy-storage devices. This is the first report of PEDOT- and PA-based carbonaceous films being used as carbon electrodes in supercapacitors.