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observed in classical Li-ion cells, where the electrolyte resistance stays rather stable upon cycling. The viscosity of the electrolyte containing polysulfides increases notably with the increasing polysulfides concentration, with viscosities of 210-2 Pa.s and 810-2 Pa.s at low shear rate (1 s- 1), for 0.1 M and 1.0 M solution of equivalent Li2S4 species, respectively†. However, the electrolyte displays a thixotropic behavior, i.e. a decrease of viscosity under high shear rate. In other words, viscosity without outflow (which represents the behavior during the battery operation) must be then higher, as the one obtained under the shearing. This non-Newtonian behavior may indicate some organization of the ionic species during the resting period with the formation of physical cross-linking. Then, the dissolution of the polysulfides in the electrolyte largely increases the viscosity and a remarkable increase of the electrolyte resistance is expected, weakly mitigated by the increase of the charge carrier number. An electrolyte resistance evolution recorded during initial cycle is shown on Figure 6-16. Such evolution is very similar to the one presented in some reports, where EIS was applied upon Li/S batteries operation132,213,214. Figure 6-16. Electrolyte resistance evolution during the initial cycle, together with the voltage profile. R’max and R”max corresponds to the points where the electrolyte resistance reaches the highest value during discharge and charge, respectively. The red dashed line indicates the level of the initial electrolyte resistance, without polysulfides inside. The green dashed line indicates the level of a maximum resistance during charge. During initial discharge, the resistance is increasing and reaches maximum at the point (marked as R’max) where formation of solid Li2S starts to occur. According to the literature, the little dip † Viscosity measurements performed on ‘catholyte’ solutions, with varying Li2S4 concentrations (0.1 M and 1.0 M) in 1M LiTFSI in TEGDME/DIOX 1/1 vol electrolyte. Chapter 6: EIS and low temperature studies 210PDF Image | Accumulateur Lithium Soufre
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