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Figures S2 and S3 show the additional data gathered from the variable current experiment (Fig. 1) and a zoomed in view of the Cl2 concentration during the 25 and 50 mA/cm2 cycling steps. We see that during the initial steps of cycling there are small perturbations in the amount of Cl2 detected. These line up well with the high states of charge (SOC) during cycling, particularly in the 25 mA/cm2 step. This indicates low level gas generation was occurring before the 10 mA/cm2 step. To explain the reasons for the increased generation of Cl2 at the 10 mA/cm2 cycling step we consider the voltages of the PE and NE as determined by the Pt reference electrode (Fig. S2b and c). As discussed in the main body of the paper, due to kinetic limitations the NE experiences significant negative polarization during the initial minute of the charging step. The voltage only experiences a slight negative shift over the remainder of the step. The PE experiences a relatively small initial shift in voltage to overcome kinetic limitations and its voltage grows during charging as a result mass transport limitations as the cell reaches higher SOCs. At higher current densities, the NE experiences more polarization (Fig. S2c). This difference in polarization is particularly evident in the 100 mA/cm2 versus 10 mA/cm2 data. This trend is reversed in the PE (Fig. S3b) where the polarization increases at lower current densities. Thus, during cycling at higher current densities we are increasing the polarization of the NE, increasing the contribution that the NE has toward cell voltage during charging. This reduces the amount of voltage increase that the PE needs to experience for the cell to reach its limit for the end of charging. At the lowest current density of 10 mA/cm2, the NE experiences less polarization and contributes less to the cell voltage. This allows the PE to experience a larger voltage increase before the cell voltage reaches the voltage limit. At the 10 mA/cm2 step this generates large enough voltages for enough time to generate concentrations of Cl2 between 3 and 4%. 21PDF Image | Chlorine Gas Generation in Mixed-Acid Vanadium Redox
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