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to a cycle. Interestingly, during the electron charge-discharge cycles two plateaus at c.a. -1.1 V and 0.9 V in Ew voltage curves were observed, in agreement with the processes recorded in the CV (Figure S9). During the experiment, the threshold value of -1.54V in discharge was reached, however the 1.38V threshold was slowly reached over the 81 cycles (Figure S9). Concurrently, this phenomenon can be compared to the CE of the battery. The efficiency was calculated on the basis of the overall cell capacity, or Q for charge-discharge of Qtheo = 0.317 mA.h (Figure 3c, purple). As shown by the green trace, the CE was almost constant and close to 100% until the 80th cycle, with a constant full capacity Q = Qtheo for two-electrons cycling. Then a drastic drop in Q discharge with an irrecoverable capacity loss of 84% between cycles 80 and 83 was observed. This corresponded to a decrease in CE in the 82nd cycle and suggested the end of our system’s life. A control CV after the incriminated 81st cycle clearly showed deterioration of our catholyte formation process, indicating the instability of the C●++ state under these stressing cycling conditions (Figure S12). Upon scanning toward the cathodic region, the appearance of a second oxidation event was observed, which was thought to be a result from the reaction with the radical dication C●++. We hypothesized that the drop in the ip intensity of the electrochemical waves could be correlated to the consumption of C+, as well as the loss of reversibility and efficiency. Current efforts consist in improving the stability of the oxidation process over time, and rationalizing its decay to improve the properties of this carbocation. In summary, we report a new high-potential organic electrolyte for nonaqueous RFBs. Through an in-depth study of the electronic characteristics of the selected carbenium ion, we have highlighted the reversibility of two redox processes with a large potential gap. The stability of the neutral radical (C•) and radical dication (C•++) forms of nPr-DMQA+ (C+) in acetonitrile was demonstrated. The analysis of fundamental electrochemical kinetics properties allowed us to 10PDF Image | Organic Redox Flow Battery Helical Carbeniun Ion
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