期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 26, 页码 29162-29172出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c03363
关键词
single-ion electrolyte; polymer; lithium-ion batteries; high transference number; in situ syntheses
资金
- Laboratory Directed Research and Development (LDRD) program through PRJ [1006525]
- DOE Office of Science [DE-AC02-06CH11357]
- U.S. Department of Energy's Vehicle Technologies Program (DOE-VTP)
Single-ion conducting (SIC) polymer electrolytes with a high Li transference number (t(Li)(+)) have shown the capability to enable enhanced battery performance and safety by avoiding liquid-electrolyte leakage and suppressing Li dendrite formation. However, issues of insufficient ionic conductivity, low electrochemical stability, and poor polymer/electrode interfacial contact have greatly hindered their commercial use. Here, a Li-containing boron-centered fluorinated SIC polymer gel electrolyte (LiBFSIE) was rationally designed to achieve a high t(Li)(+) and high electrochemical stability. Owing to the low dissociation energy of the boron-centered anion and Li+, the as-prepared LiBFSIE exhibited an ionic conductivity of 2 x 10(-4) S/cm at 35 degrees C, which is exclusively contributed by Li ions owing to a high t(Li)(+) of 0.93. Both simulation and experimental approaches were applied to investigate the ion diffusion and concentration gradient in the LiBFSIE and non-cross-linked dual-ion systems. Typical rectangular Li stripping/plating voltage profiles demonstrated the uniform Li deposition assisted by LiBFSIE. The interfacial contact and electrolyte infiltration were further optimized with an in situ UV-vis-initiated polymerization method together with the electrode materials. By virtue of the high electrochemical stability of LiBFSIE, the cells achieved a promising average Coulombic efficiency of 99.95% over 200 cycles, which is higher than that of liquid-electrolyte-based cells. No obvious capacity fading was observed, indicating the long-term stability of LiBFSIE for lithium metal batteries.
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