Journal
NATURE ENERGY
Volume 7, Issue 2, Pages 186-193Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41560-021-00977-5
Keywords
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Funding
- US Department of Energy ARPA-E [DEAR0000389]
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Researchers have developed a new non-aqueous ternary eutectic electrolyte with a wider electrochemical stability window and lower salt concentration. By using this electrolyte, they have achieved high efficiency and capacity retention in lithium-ion batteries.
To compete with commercial organic electrolytes, aqueous electrolytes beyond water-in-salt electrolytes with a lower salt concentration of <5.0 m (mol kg(solvent)(-1)) and wider electrochemical stability window of >3.0 V are urgently needed. Here we report a 4.5 m lithium bis(trifluoromethanesulfonyl) imide (LiTFSI)-KOH-CO(NH2)(2)-H2O non-flammable ternary eutectic electrolyte that expands the electrochemical stability window to >3.3 V by forming a robust solid-electrolyte interphase. The ternary eutectic electrolyte enables Li1.5Mn2O4 || Li4Ti5O12 pouch cells to achieve a high average Coulombic efficiency of 99.96% and capacity retention of 92% after 470 cycles at an areal capacity of 2.5 mAh cm(-2), a low positive/negative capacity ratio of 1.14 and a lean electrolyte (3 g Ah(-1)). The Li loss due to the solid-electrolyte interphase formation in the initial charge/discharge cycles is compensated by an excess 0.5 Li in the Li1.5Mn2O4 cathode, which converts the Li1.5Mn2O4 || Li4Ti5O12 cell into LiMn2O4 || Li4Ti5O12 after solid-electrolyte interphase formation. The 2.5 V aqueous Li1.5Mn2O4 || Li4Ti5O12 pouch cells with practical settings demonstrate a promising approach towards safe, low-cost and high-energy aqueous Li-ion batteries. High-energy batteries require electrolytes with a wide electrochemical stability window. Building on the water-in-salt electrolyte concept, the authors develop a ternary eutectic electrolyte with substantially reduced salt concentrations that enable high-performance Li1.5Mn2O4 || Li4Ti5O12 batteries
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