期刊
ADVANCED ENERGY MATERIALS
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202302443
关键词
anion-enriched solvation sheath; diluted ethereal electrolyte; high-voltage Li metal batteries; ionic liquids; solvation structure
In this study, a diluted ethereal electrolyte with an anion-enriched solvation sheath is developed for high-voltage Li metal batteries. The electrolyte enables long-term cycling and high-rate performance.
Given the high compatibility with Li metal anodes, ethereal electrolytes have found widespread use in Li metal batteries. Unfortunately, their applications in high-voltage Li metal batteries are hampered by a limited electrochemical window. In this study, a diluted ethereal electrolyte (with Li salt concentration < 1.5 m) is developed containing 1 m lithium bis(fluorosulfonyl) imide (FSI) and 0.3 m LiNO3 in a N-methyl-N-propylpiperidinium bis(trifluoromethanesulfonyl)imide (PP13TFSI):dimethyl ether (DME) (v:v = 1:4) mixture for Li metal batteries with an aggressive high-voltage cathode via the formation of an anion-enriched solvation sheath. In contrast to high-concentration electrolytes, the formation of the anion-enriched solvation sheath in this design is facilitated by the addition of ionic liquids. Further theoretical calculations indicate that the presence of FSI- and NO3- anions in the first solvation sheath weakens the desolvation energy of the DME solvent, suggesting a faster desolvation process at the electrode interphase. Consequently, the designed electrolyte enables long-term cycling of Li || LiNi0.8Co0.1Mn0.1O2 (NCM811) full cells over 1000 cycles at a high rate of 10 C. More notably, it also allows for a long cycle life of 100 cycles under a high rate of 5 C, even with limited negative capacity to positive capacity (N/P) ratio of 1.
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