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Simulation of Mediator-Catalysis Process inside Redox Flow Battery

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Abstract

Reduction of alkali or alkaline earth metal chlorates to chlorides is of great interest for its use as the positive-electrode process of a redox flow battery in view of very large theoretical estimates of its specific charge per solution unit mass or volume owing to high solubilities of the reagent and the product as well as to the six-electron transfer per one chlorate ion. Such use of this oxidizing agent requires overcoming a fundamental difficulty: the non-electroactivity of the chlorate anion at electrodes in the required potential range. Promising approach to the implementation of this process is using a mediator catalysis based on an Ox/Red redox couple which has a high positive potential and a fairly large exchange current, while its Red form is able reacting chemically in solution with the chlorate anion, reducing it to the chloride anion, with regeneration of the Ox form. Such a mediator cycle can be implemented in the positive part of the flow battery based on multiple pumping of the solution from the reservoir through the discharging device for the electrochemical conversion of the Ox form of the redox couple into the Red component, with the electricity generation. Meanwhile, the chemical stage, i.e., the reaction of the chlorate anion with the Red form takes place inside the reservoir. Theoretical analysis of the functioning of such a system under galvanostatic mode has been performed in this study. Time-variation of the component concentrations and the electrode potential has been predicted. Two different scenarios for the system evolution have been revealed, depending on the relationship between the passing current and its critical value. Treatment of experimental data for the variation of the electrode potential and the redox-couple component (Ox or Red) concentration are proposed, in order to establish the values of the system parameters including the critical current value and the rate constant of the chemical stage of the process.

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This work was supported by the Russian Science Foundation, grant no. 20-63-46041.

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  1. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences, 119071, Moscow, Russia

    M. A. Vorotyntsev & P. A. Zader

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Vorotyntsev, M.A., Zader, P.A. Simulation of Mediator-Catalysis Process inside Redox Flow Battery. Russ J Electrochem 58, 1041–1056 (2022). https://doi.org/10.1134/S1023193522110118

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