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Chapter 1: Literature review used in so-called ‘all-liquid cell’, i.e. ‘catholyte’, where sulfur active material is directly dissolved in the electrolyte, in the form of Li2Sx (x = 6 or 8)126 or Li2S5164. Phosphorus pentasulfide (P2S5) was reported as an additive by Liang et al.181. P2S5 prevents the formation of solid Li2S on both positive and negative electrodes. Thus, during discharge, no solid phase is formed on the positive electrode, eliminating the risk of passivation. It can also get reduced on the metallic lithium surface by forming Li3PS4, which may suppress polysulfide shuttle phenomenon and irreversible losses of active mass (because of Li2S precipitation on lithium). This additive, however, is much less studied and utilized as compared with the most popular LiNO3, probably to its sensitive manipulation. As previously discussed (section 1.3.1.c), an important parameter that should be taken into consideration is the electrolyte/sulfur ratio, since it was proved to influence both cyclability and capacity105,106,109,125. Electrolyte added in a large excess may provide better solubility of sulfur and polysulfides species. However, it can also strongly decrease the practical energy density of the cell123, and may also be responsible for fast capacity fading during initial few cycles (Figure 1-18). In the work of Ding et al.125, this capacity fading was attributed to the large amount of electrolyte, which acts as a polysulfides reservoir, preventing further utilization of this lost active mass. Lower amount of electrolyte was demonstrated to provide more stable cycling, however, at much lower sulfur utilization. Thus, the literature rather refers to an ‘optimized S/E’ ratio, which may be different for each system studied. Therefore, different values can be found in the literature (50 gsulfur Lelectrolyte-1, or ~ 100 gsulfur Lelectrolyte-1 for example105,106). Figure 1-18. Capacity retention of a S/C composite electrode (S/C = 2/1) with a sulfur loading of 2.4 mg cm-2, cycled with different electrolyte volumes at a current density of 57 μA cm-2 125. 36PDF Image | Accumulateur Lithium Soufre
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