Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 117, Issue 40, Pages 20509-20516Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp407158y
Keywords
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Funding
- Advanced Low Carbon Technology Research and Development Program (ALCA) of the Japan Science and Technology Agency (JST)
- Technology Research Grant Program of the New Energy and Industrial Technology Development Organization (NEDO) of Japan
- Grants-in-Aid for Scientific Research [23245046] Funding Source: KAKEN
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A series of equimolar mixtures of Li salts (LiX) and glymes (triglyme (G3) and tetraglyme (G4)), [Li(glyme)]X with different anions (X: [N(SO2C2F5)(2)] = [BETI]; [N(SO2CF3)(2)] = [TFSA]; [CF3SO3] = [OTf]; BF4; NO3), were used as electrolytes to study the anionic effects of [Li(glyme)]X on the performance of lithium-sulfur (Li-S) batteries. The dissolution of lithium polysulfides (Li2Sm), which are discharge products of elemental sulfur, was significantly suppressed in the solvate ionic liquid (IL) electrolytes, as seen in [Li(G(4))][BETI] and [Li(glyme)][TFSA], wherein all of the glymes participated in the formation of the complex cation [Li(glyme)](+). It was found that NO3 anions were irreversibly reduced at the composite cathode during discharge and BF4 anions formed unexpected byproducts through a chemical reaction with the polysulfide anions. Successful charge/discharge of Li-S cell could not be performed in [Li(glyme)]X in the presence of these anions because of the undesired side reactions. The solvate IL [Li(G4)][BETI] was found to be electrochemically stable in the Li-S cell and allowed a stable operation with a capacity of 600700 mAh.g(-1) and a Coulombic efficiency of 98.5% over 100 cycles, similar to that achieved by [Li(glyme)][TFSA]. In contrast, the Li-S cell with a concentrated electrolyte solution, [Li(G3)][OTf], showed a much lower capacity and Coulombic efficiency.
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