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250 200 150 100 50 0 -50 -100 -150 ref sim charge discharge 1.5 2.0 2.5 3.0 Voltage vs. Li/Li+ / V Figure 5.19: Cyclic voltammetry data compared to experimental results. Sweep rate: 25μV·s−1. experimental data was recorded from a cell of a different batch than the data used for calibration. The performance of that batch was slightly better, therefore the total capacity of the reference cell is expected to be larger. Second, the position of the ca- thodic peaks is shifted compared to the reference, which most likely can be explained by a flaw in the calibration already discussed above: It is impossible to obtain exper- imental data of a quasistatically slow galvanostatic discharge. Lacking more precise information about the composition of the overpotential, the thermodynamics were cal- ibrated using the midpoint between the charge and discharge voltage of a finitely fast discharge in Fig. 5.13. The thermodynamically correct voltage, however, is possibly off-center and indeed, judging based on Fig. 5.19, this seems to be the case for this system. Third, the shape of the peaks does not match precisely. In the experimen- tal data set, both the charge peak and the lower discharge peak extend into a “tail”, blurred over several hundred mV. As already mentioned in the discussion of Fig. 5.18, these tails are most likely caused by sulfur that is more strongly (chemically) bound to the electrode matrix and thus only accessed at higher overpotential during both charge and discharge – a phenomenon which is not included in the model. 119 Current / μAPDF Image | Lithium-Sulfur Battery: Design, Characterization, and Physically-based Modeling
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