The self-discharge behavior of organic electrodes and symmetric devices for sustainable energy storage, composed of electrodes containing a thin layer of polypyrrole coated onto a high surface area cellulose matrix, has been studied for the first time using different electrode sizes and electrolytes. Experimental data from open circuit measurements of the individual electrode potentials of charged symmetrical two-electrode energy storage devices as a function of time were evaluated based on three different self-discharge models. This evaluation clearly showed that the self-discharge process of the positive electrode is governed by a previously undetected activation-controlled faradaic reaction while the self-discharge of the negative electrode is due to diffusion controlled oxidation involving oxygen dissolved in the electrolyte. Potentiostatic three-electrode measurements and spectroelectrochemical experiments also showed that protons as well as maleimide were released from positively polarized polypyrrole electrodes. These new findings clearly show that the self-discharge of the cells originate from two different types of reactions on the positive and negative electrodes and that the main contribution to the self-discharge of the cells comes from an activation controlled reaction involving the positive electrode. These results provide an improved understanding of polypyrrole based devices and also yield new possibilities for the development of stable conducting polymer system for energy storage applications.
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