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interpreted as the average thickness of the insulating layer at the time when electrons can no longer tunnel through its thinnest segment. This paragraph only deals with the calibration of ξ1 and ξ2; the formation of the passivating film is analyzed in more detail below, cf. Fig. 5.27 on page 128. Enthalpy of formation of dissolved species. In order to correct the enthalpies of formation of the dissolved polysulfides for the effect of the liquid electrolyte, the gas- phase thermochemistry values taken from Ref. [143] are shifted by a fixed offset ∆g0. The offset is determined as follows: 1. Choose fast rate constants. 2. Starting from a fully charged cell, simulate a discharge with a very slow rate and plot voltage vs. capacity (see Fig. 5.13). 3. Adjust the offset until the lower plateau voltage for charge and discharge is roughly centered between the charge and discharge branches of the reference data. The actual voltage will change when calibrating the reaction rates, but the center is virtually not affected. Unfortunately, very slow discharges are difficult to obtain experimentally – or rather difficult to interpret since the discharge due to the externally applied current mixes 3.2 3.0 2.8 2.6 2.4 2.2 2.0 1.8 Figure 5.13: Parameter variation: Enthalpy of formation of the dissolved polysulfides. ∆g0 denotes the fixed offset to gasphase thermochemistry data. Reference data: discharge at C/50, charge at C/20. The different simulations may alternatively be interpreted as different electrolytes. ref 210 kJ/mol 215 kJ/mol ∆g0 = 220 kJ/mol 225 kJ/mol 230 kJ/mol 110 0 50 100 150 200 250 300 Capacity / Ah/kgS Cell voltage / VPDF Image | Lithium-Sulfur Battery: Design, Characterization, and Physically-based Modeling
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