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mixture at the end of discharge can be estimated. Taking into account the stoichiometry of the two reactions (S42- + 2 e- → 2 S22- and S42- + 6 e- → 4 S2-), the molar ratio can be determined, and the mixture might then be composed of about 40% of Li2S and 60% of Li2S2, without excluding the existence of other polysulfides in a small amount. A schematic illustration on Figure 5-13 summarizes the proposed mechanisms arising from XRD data treatment. Figure 5-13. Proposed mechanism for Li2S/Li2S2 formation upon discharge. The low voltage plateau can be divided into two parts, which do not follow the same mechanisms: • during the first step, Li2S is produced with an efficiency close to 100 % • during the second step, Li2S is produced with a much lower efficiency, of about 13 %, calculated with equation (19): 2 0 3.55Kh 3 = 12&− 2 30 + 2 303 3.5 5Kh + 8.1 5Kh (19) 12 & − 4 & − while Li2S2 is predominantly formed with an efficiency close to 87 %. We clearly prove that Li2S4 is directly reduced to Li2S with 100 % of efficiency at the beginning. This behavior could be associated with the weak stability of Li2S2 compound241. Afterward, the efficiency decreases dramatically down to 13 %. This large modification in the reduction mechanism of S42- (Li2S or Li2S2 formation) could be related to the passivation of the electrode with the formation of insulating Li2S layer, which Chapter 5: In situ and operando XRD 178PDF Image | Accumulateur Lithium Soufre
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