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| - Deciphering the Origin of High-Order Periodic and Aperiodic Cyclic VoltammetricResponses During Oxidation Processes on Platinum
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| - We report cyclic voltammograms of the hydrogen electrooxidation reaction on a rotating Pt ring electrode indiluted electrolytes that are either aperiodic or possess a period which is a multiple of the period of thecycling voltage. The complex voltammetric responses are experimentally studied in two electrolytes withdifferent compositions of the base electrolyte (and thus different conductivity) as a function of the positiveturning point of the applied voltage. The behavior can be rationalized in terms of the interaction between theinhibition of H2 oxidation by Pt−oxides, the roughening of the electrode due to oxide reduction and itssubsequent smoothing as well as a nonnegligible uncompensated voltage drop through the electrolyte. Theproposed mechanism is translated into a mathematical model consisting of a set of four ordinary differentialequations. The model indeed captures the main experimental findings. Since the principle ideas do not dependon the specific kinetics of the oxidation reaction under investigation, the mechanism should be operative ina variety of electrochemical systems. In particular, we suggest that it may underlie the complex cyclicvoltammograms observed during many oxidation reactions of small organic molecules.
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