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density of 5 mA/cm2 up to a capacity limit of 10 mAh was performed, followed by discharging to a voltage limit of 0.8V. After the formation step described above, the open-circuit voltage (OCV) of the cell was 1.7V, close to the theoretical value, after charging to 10% state-of-charge (SOC). Reversible cycling was observed, with a coulombic efficiency of 96-92% over the first 50 cycles. In comparison, beaker-type cells without either the Nafion membrane or the organic solvent accumulator exhibited a coulombic efficiency of less than 50%, as shown in the SI. For the flat cells, after about 50 cycles a step in charge voltage emerged at high SOC. The same feature is seen in the plot of cathode-reference potential vs capacity, Figure 2c, showing that it is related to a positive electrode reaction. We attribute this feature to the onset of OER at the cathode, which is expected if there is a loss of working ClO2/ClO2- resulting in OER when the cell is “overcharged.” The voltage plateau at 1.9-2.O V (vs Ag/AgCl) in Figure 2C is considerably higher than the theoretical OER potential in a near-neutral solution of 0.6V (vs Ag/AgCl). However, the existence of a high kinetic overpotential for OER at the surface of carbon electrodes is well-known. We speculate that loss of ClO2/ClO2- may have occurred due to incomplete blocking of chlorite crossover to the Zn electrode, partial disproportionation of ClO2 in the electrolyte, or possibly leakage of ClO2 from the cell. These loss mechanisms may be further mitigated by improvements in cell design, including implementation in half-flow or flow-battery designs. Treating the cell in Figure 2 as the power- generating stack of a flow battery, the ClO2 product could be stored in a tank and circulated to the positive electrode. The zinc negative electrode is likely stationary, but circulation of the alkaline electrolyte may have similar advantages to those in Zn-air cell designs [18] such as suppression of metal dendrites. The independent scaling of tank storage and stack power generation that is inherent in flow- battery designs means that the system could be tailored to address storage needs over a wide range of durations, including long-duration storage [2]. Finally, the rapid redox kinetics combined with stability of ClO2 in the liquid phase at ambient pressures below ~11°C suggests that chlorite based batteries may be especially attractive for low temperature stationary storage, including Arctic, Antarctic, or extraterrestrial applications. 6PDF Image | Reversible Chlorite Chlorine Dioxide Anion Redox Storage
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