Composite films consisting of poly(3,4-ethylenedioxythiophene) (PEDOT) and graphene oxide (GO) were electrochemically polymerized by electrooxidation of EDOT in ionic liquid (BMIMBF4) onto flexible electrode substrates. Two polymerization approaches were compared, and the cyclic voltammetry (CV) method was found to be superior to potentiostatic polymerization for the growth of PEDOT/GO films. After deposition, incorporated GO was reduced to rGO by a rapid electrochemical method of repetitive cathodic potential cycling, without using any reducing reagents. The films were characterized in 3-electrode configuration in BMIMBF4. Symmetric supercapacitors with aqueous electrolyte were assembled from the composite films and characterized through cyclic voltammetry and galvanostatic discharge tests. It was shown that PEDOT/rGO composites have better capacitive properties than pure PEDOT or the unreduced composite film. The cycling stability of the supercapacitors was also tested, and the results indicate that the specific capacitance still retains well over 90% of the initial value after 2000 consecutive charging/discharging cycles. The supercapacitors were demonstrated as energy storages in a room light energy harvester with a printed organic solar cell and printed electrochromic display. The results are promising for the development of energy-autonomous, low-power, and disposable electronics.
Harvesting micropower energy from the ambient environment requires an intermediate energy storage, for which printed aqueous supercapacitors are well suited due to their low cost and environmental friendliness. In this work, a systematic study of a large set of devices is used to investigate the effect of process variability and operating voltage on the performance and stability of screen printed aqueous supercapacitors. The current collectors and active layers are printed with graphite and activated carbon inks, respectively, and aqueous NaCl used as the electrolyte. The devices are characterized through galvanostatic discharge measurements for quantitative determination of capacitance and equivalent series resistance (ESR), as well as impedance spectroscopy for a detailed study of the factors contributing to ESR. The capacitances are 200–360 mF and the ESRs 7.9–12.7 Ω, depending on the layer thicknesses. The ESR is found to be dominated by the resistance of the graphite current collectors and is compatible with applications in low-power distributed electronics. The effects of different operating voltages on the capacitance, leakage and aging rate of the supercapacitors are tested, and 1.0 V found to be the optimal choice for using the devices in energy harvesting applications.
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