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0.022 mV/s and 0.015 mV/s, respectively. The NE voltage decreases by 200 mV in the first 45 seconds of stage one then only decreases another 50 mV over the rest of charging. Previous research suggests that the NE causes an initial spike in cell polarization while the PE dominates changes in the cell voltage over time due to mass transport limitations. The posolyte reactions in the MA system are experimentally observed to be diffusion controlled while the negolyte reactions are shown to be kinetically limited.10 Our study appears to confirm that the PE is more likely to become severely mass transport limited as charging of the cell continues while the NE will be kinetically limited during the entire charging step. This would explain why most of the NE’s polarization occurred in the first minute of charging, as it was necessary to drive the reaction kinetically. In contrast, the PE’s polarization occurred gradually over the charging step as mass transport conditions became less ideal. One might expect higher mass transport limitations at higher current densities, yet miniminal Cl2 generation is observed above 10 mA/cm2. A more detailed explanation of the intersection between polarization at both electrodes and mass transport limitations is provided in the Supporting Information. Mass transport limitation of the PE coincides with the onset of Cl2 generation during charging. In a mass transport limited system held at constant current, the voltage increases rapidly until a new reaction becomes viable and can contribute to the generation of current.16 This sharp increase in voltage is observed in the transition region and occurs at the onset of Cl2 generation, suggesting that V4+ oxidation is no longer the preferred reaction. In stage two the voltages have slopes that level off indicating the PE has become kinetically limited again and a new reaction has been activated at the increased voltage. Increased observed Cl2 that coincides with this transition suggests the new reaction is electrochemical formation of Cl2 gas. 7PDF Image | Chlorine Gas Generation in Mixed-Acid Vanadium Redox
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