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III.B.6 Development of High-Energy Lithium Sulfur Cells Johnson – NETL, Wang – PSU 1000 mAh/g, as shown in Figure III - 69a. Its low viscosity also leads to low cell polarization. ANL-E-4 fluorinated ether based electrolyte was shown to give high initial capacity and a decreased polysulfide shuttle effect. Several additives for this electrolyte were tested. Addition of 0.2M LiBr was found to help stabilize the capacity of cells with PSU-3 sulfur cathodes, Li foil anodes, and the new fluorinated electrolyte at around 800 mAh/g for 50 cycles, but did not improve the efficiency above ~95%; this is shown in Figure III - 69b. With an eye toward better utilizing Li2S formed at the end of the discharge process, anion 1400 1200 1000 800 600 400 200 receptors – organic molecules which can form a strong coordination bond between the S2- anion and the electron deficient atom such as B and Al – were also tested as electrolyte additives. Triethyl borate was found to increase coulombic efficiency, albeit with relatively low capacity retention. Finally, LiNO3 was also tested in combination with the fluorinated electrolyte and was found to significantly improve efficiency, but not capacity retention, as it is not believed to prevent polysulfide dissolution. S=5.20mg/cm2 S=5.60mg/cm2 S=4.95mg/cm2 0 0 5 10 15 20 25 30 35 40 1400 1200 1000 800 600 400 200 100 80 60 40 20 Cycle Number (a) Several tests were also conducted to better understand the mechanism by which LiNO3 improves battery performance. By testing cells with varying electrolytes having LiNO3 concentrations, it was determined that LiNO3 is used up during cycling and thus cannot provide long-term efficiency improvement, and furthermore, that it cannot prevent long-term loss of capacity. It was also found, by moving Li anodes from cells cycled in LiNO3-containing electrolyte to cells with LiNO3-free electrolyte, that LiNO3 does not appear to form a very stable protective layer on the anode. Pouch Cell. Initially, pouch cell designs were planned and optimized, particularly with regard to the N/P ratio of cells. It was found that in order to achieve a cell-level capacity of 200 Wh/kg, the specific capacity must be 800 mAh/g S with an N/P ratio of 5.2, or over 900 mAh/g S with an N/P ratio of 2.0. This and other design factors were taken into account during pouch cell design. Numerous pouch cells were fabricated and tested. Cells with Li foil anodes, PSU-3 cathodes, and baseline electrolyte with 0.4M LiNO3 proved to have poor capacity, stability, and efficiency. Cells with 0.34 Ah designed capacities showed only a 0.2 Ah after 50 cycles, with an efficiency of only 40% by that point. Cells with 1.5 Ah designed capacity had at most a 1.19 Energy Storage R&D 84 FY 2013 Annual Progress Report Discharge capacity Coulombic efficiency 00 0 10 20 30 40 50 Cycle Number (b) Figure III - 69: Cycling of cells with PSU-3 cathodes and a) PSU-E-5 electrolyte or b) ANL-E-4 fluorinated ether electrolyte with 0.2M LiBr Discharge Capacity (mAh/g) Discharge Capacity (mAh/g) Coulombic Efficiency (%)PDF Image | Advanced Battery Development
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