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Crystals 2022, 12, x FOR PEER REVIEW 6 of 10 6 of 9 Figure 4. The cyclic voltammetry (CV) of LCO||Li cells from 3.0–4.6 V with (a) DES-1, (b) DES-2, Figure 4. The cyclic voltammetry (CV) of LCO||Li cells from 3.0–4.6 V with (a) DES-1, (b) DES-2, aand((cc))DES--3..((d))Theelectrochemiicalliimpedanccespecttrroscopy((EIIS))of LCO|||LLiicceellslswitithhtthrreee DESSeelleeccttrrollyttessbefforrecyclle.. Crystals 2022, 12, 1290 Strategy PVDF/PVAC-Based CPE Sulfonamide-based electrolyte 0.2% ATCN LiTFSI-P13FSI-TTE SN-DLi-FEC 10% MSM + DMC/FEC/HFE Dual-salt Deep Eutectic Electrolyte Voltage 3.0–4.5 3.0–4.55 3.0–4.5 3.0–4.3 3.0–4.4 2.75–4.45 3.0–4.45 3.0–4.45 3.0–4.6 Rate 0.5 C 0.3 C 1 C 0.5 C 0.5 C 200 mA/g 0.5 C 2 C 1 C Cycling Retention 200 85% 200 89% 200 91% 350 80% 200 85% 300 87.1% 200 94% 500 72% 200 70% Ref. [39] [40] [41] [26] [27] [25] This work The long cycling performance of DES electrolytes was further evaluated in LCO||Li Figure 5a,b demonstrates the rate performance of three DES electrolytes; the DES-1 cells under 3.0–4.45 V and 3.0–4.6 V. As shown in Figure 5c, the cell with DE−1S-2 delivers a delivers a reversible capacity of 170.9, 168.6, 162.8, 157.9, and 152.2 mAh g at 0.1 C, 0.2 high capacity of 111.5 mAh g−1 after 600 cycles at 0.5 C under 3.0–4.45 V, whic−h1 is higher C, 0.5 C, 1 C, and 2 C, respectively, and the capacity recovers to 170.3 mAh g after re- than DES-1 of 97.9 mAh g−1 and DES-3 of 77.5 mAh g−1. In contrast, carbonate-based turning to 0.1 C. DES-2 exhibits better rate performance than DES-1, with a relatively high electrolytes exhibit a relatively low initial capacity of 1−153.9 mAh g−1 and suffer from rapid capacityof188.3,181.1,171.9,165.8,and159.2mAhg ,at0.1C,0.2C,0.5C,1C,and2C, capacity decay. Figure 5f–h shows the voltage–capacity cu−r1ve of three DES electrolytes respectively, and the high capacity recovers to 187.8 mAh g after returning to 0.1 C. In with different cycles under 3.0–4.45 V. The results demonstrate that the initial Coulombic addition, the DES-3 delivers a reversible capacity of 178.8, 175.4, 169.8, 164.8, and 158.3 efficien−1cies of DES-1, DES-2, and DES-3 are 87.9%, 91.2%, and 63.1%, respectively. Moreover, mAh g at 0.1 C, 0.2 C, 0.5 C, 1 C, and 2 C, respectively, and the capacity recovers to 177.7 DES-2 −e1xhibits a lower polarization during cycling. Moreover, the cells display outstanding mAh g after returning to 0.1 C. By contrast, carbonate-based electrolyte only delivers a cycling stability, with the reversible capacity of 112.1, 110.3, and 1−105.0 mAh g−1 for DES-1, reversible capacity of 174.8, 170.4, 166.5, 161.1, and 153.6 mAh g at 0.1 C, 0.2 C, 0.5 C, 1 DES-2, and DES-3 after 700 cycles at 2 C, respectively (Figure 5d), which is much higher than C, and 2 C, respectively. The better rate performance of DES-2 is mainly attributed to the carbonate-based of 54.8 mAh g−1. Notably, DES-2 exhibited the highest average Coulomb higher Li+ transference number, which facilitates the rapid Li+ migration and reduces cell efficiency of 99.6%, higher than DES-1 at 97.6% and DES-3 at 99.4%. To further demonstrate polarization. the good oxidation resistance of DES, LCO||Li cells were cycled at 3.0–4.6 V. The DES-3 delivers the highest initial discharge capacity of 208.9 mAh g−1 at 1 C. In addition, all DES electrolytes can be stably cycled for 500 cycles at 1 C and under the voltage of 3.0–4.6 V (Figure 5e,i–k). The carbonate-based only delivers a reversible capacity of 89.7 mAh g−1 after 200 cycles at 3.0–4.6 V and 1 C. Consequently, the dual-salt DES electrolyte exhibits excellent cycling performance in high voltage LCO||Li cells (Table 2). Table 2. A comparison with some previous reports on cycling performance.PDF Image | Non-Flammable Dual-Salt Deep Eutectic Electrolyte
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