Journal
ELECTROCHIMICA ACTA
Volume 368, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2020.137535
Keywords
Lithium metal batteries; Mixed electrolytes; Ionic liquids; Density functional theory
Categories
Funding
- National Natural Science Foundation of China [51972180]
- Key Research & Development Project of Shandong Province [2019GGXI02070]
- Program for Scientific Research Innovation Team in Colleges and Universities of Jinan [2018GXRC006]
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The ionic liquid [MEMP][TFSI] can significantly improve the cycling performance of lithium metal batteries, increasing effective cycle number by as much as 84.6%. With [MEMP][TFSI] in the electrolyte, the Li metal anode shows low and stable polarization, excellent cycle performance, uniform Li deposit, thinner Li layer, and low interfacial impedance. The addition of [MEMP][TFSI] enhances the interaction between Li and oxygen, as well as the charge transfer from Li, leading to more stable battery cycling performance.
Metallic lithium (Li) has been researched extensively in recent years due to its high theoretical specific capacity and its extremely low redox potential. However, uncontrolled Li dendrites growth during the charging process can lead to safety problems and shortens the life of lithium metal batteries (LMBs). Our recent work has discovered that an ionic liquid (IL), namely, N-methyl, (2-methoxyethyl)-pyrrolidinium bis(trifluoromethylsulfonyl)imide ([MEMP][TFSI]), can significantly improve the cycling performance when added into the conventional electrolyte. Compared with LMBs with no ionic liquids (ILs), those with mixed electrolytes containing [MEMP][TFSI] can increase the effective cycle number by as much as 84.6%. Li metal anode with mixed electrolytes containing [MEMP][TFSI] presents low and stable polarization, excellent cycle performance, uniform Li deposit, and thinner Li layer, as well as low interfacial impedance. Density functional calculations are carried out and demonstrate that the addition of [MEMP][TFSI] enhances the interaction between Li and oxygen as well as the charge transfer from the Li, which prevents Li deposit growth at the Li metal anode surface and also enables a more stable battery cycling performance. The key findings of this study provide a useful method to research the molecular engineering of electrolyte components by experiments and by density functional theory (DFT) calculations. (C) 2020 Elsevier Ltd. All rights reserved.
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