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Chapter 5: In situ and operando XRD Figure 5-14. Charge process: investigation of Li2S consumption and charging mechanism. Upon charge, the oxidation of both Li2S and Li2S2 products occurs. During the first step, using the recorded evolution of Li2S (111) peak area, 75 % of Li2S amount that was formed at the end of discharge, is oxidized (equation (20). /&#* #$&# -A 2 30 #B Bh& & -A Bh& A $ B B&7 -A !h#$%& = 219 = 0.25 (20) /&#* #$&# -A 2 30 #B Bh& & -A !h#$%& 864 This amount of oxidized Li2S corresponds to: • If we consider the reaction pathway 8S2- → 2S42- + 12e-, 75 % of Li2S conversion is associated with 6.1 mAh (0,758.1 mAh, i.e. the amount of charge related to Li2S formation during prior discharge). As 10.5 mAh (refer to Figure 5-14) permit to oxidize both Li2S and Li2S2 during the first step of the charge process, the oxidation of Li2S2 corresponds to 4.4 mAh, i.e. 54 % of Li2S2 is oxidized (O.O PQR 100 %) 1.M PQR • If we consider the reaction pathway 2S2- → S22- + 2e-, 75 % of Li2S conversion is associated with 4.3 mAh. As 10.5 mAh (refer to Figure 5-14) permit to oxidize both Li2S and Li2S2 during the first step of charge process, the oxidation of Li2S2 to Li2S4 (4S22- → 2S42- + 4e-) corresponds to 6.2 mAh. Since the capacity of 2.82 mAh corresponds to the exchange of one electron, 2.2 electrons would then be exchanged through this reaction pathway, which would correspond to 55 % of Li2S2 oxidized to Li2S4 (i.e. 2.2 electrons over the 4 electrons needed for the complete reappearance of Li2S4). Whatever the charging process (the direct oxidation of Li2S to Li2S4 or the oxidation of Li2S to Li2S2), Li2S seems to be oxidized during the first step at higher rate than Li2S2. During the 180PDF Image | Accumulateur Lithium Soufre
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