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LiNO3 in DOL/DME (Supplementary Fig. 4b), E_G2 (Supplementary Fig. 4a), and E_G2_0.5 M Li2S4 (Supplementary Fig. 4c). All cells were tested at 0.3 C rate and 30 °C. After 500 cycles, the lower discharge plateau corresponding to reaction [3] totally disappeared and the capacity decay was almost continuous in the cells using E_G2 and E_DOL/DME, suggesting the surface pathway of reaction [3] should prevail in these two cells to result in a parasitic loss of surface area by the passivation of Li2S during cycling. However, the length of the lower discharge plateau has a minimal change for the cell using E_G2_0.5 M Li2S4. This indicates that the presence of excess Li2S4 in the electrolyte is helpful to stabilize the lower discharge plateau during cycling. Dependence of sulfur utilization efficiency on the content of Li2S4 in electrolyte To further correlate the interplay between Li2S4 content in the bulk electrolyte and the reduction efficiency of solid Li2S4 under lean electrolyte conditions, ACFC_Li2S8 was prepared by preloading 30 μL of 1 M Li2S8 (sulfur mass loading: 6.06 mg cm−2) into ACFC. Fig. 2a shows typical discharge curves of Li ǀ E_G2_x M Li2S4 ǀ ACFC_1 M Li2S8 with an E/S ratio of 3.0 mLE gs_cathode−1 at 0.12 mA cm−2 and 30 °C, where gs_cathode represents the weight of sulfur in cathode (not including those in electrolyte). The achievable discharge capacity shows a strong correlation with the concentration of Li2S4 in the electrolyte. The cell using E_G2_0.5 M Li2S4 shows a significantly high capacity of 1520 mAh gs_cathode−1 based on preloaded Li2S8 and1268 mA gs_total−1 based on the total sulfur loading (including those pre-loaded in ACFC and those in the electrolyte) at an elevated discharge potential. In contrast, limited capacities of < 400 mAh gs_cathode−1 were observed for lower (<0.5 M) and higher concentrations (0.75 M) of Li2S4, indicating that an optimal concentration of Li2S4 in the bulk electrolytes is required to reduce preloaded Li2S8 to solid Li2S4 and the following Li2S effectively. This is the first time that nearly 100% solid Li2S4 reduction has been reported for Li-S coin cells with high sulfur loadings and lean electrolytes. Cells were both halted near the nucleation stage using the couple of E_G2ǀACFC_Li2S8 or E_G2_0.50 M Li2S4ǀACFC_S8 in the Fig. 2b and Supplementary Fig. 5 indicate that both the starting sulfur material and the 0.5 M Li2S4 content in electrolyte have a remarkable impact on the sulfur utilization. The cell using E_DOL/DME presents a lower discharge plateau, at 1.85 V, and a limited discharge capacity of 897 mAh gs_cathode−1, far below that of the cell using E_G2_0.50 M Li2S4. Moreover, bulk electrolytes with 2 M [S] were made from 0.25 M Li2S8 and 0.33 M Li2S6 and examined, as shown in Fig. 2c. Interestingly, the cell using 0.33 M Li2S6 shows the absence of a lower discharge plateau. However, the cell using 0.25 M Li2S8 presents a specific capacity of 1884 mAh gs_cathode−1, indicating that sulfur from the bulk electrolyte of 0.25 M Li2S8 migrated into the ACFC and contributed to the total capacity due to the concurrent reduction of Li2S8 from the bulk electrolyte and the ACFC, where the intermediate reduced species of Li2S6 are not supposed to generate from E_G2_0.25 M Li2S8; otherwise, it would exhibit no lower discharge plateau, as did the cell using E_G2_0.33 M Li2S6. Page 5 of 24PDF Image | A lithium-sulfur battery with a solution-mediated pathway
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