Research ArticleELECTROCHEMISTRY

Upgrading traditional liquid electrolyte via in situ gelation for future lithium metal batteries

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Science Advances  05 Oct 2018:
Vol. 4, no. 10, eaat5383
DOI: 10.1126/sciadv.aat5383
  • Fig. 1 Mechanism, structure, and characterization of GPE.

    (A) Schematic model of the polymerization mechanism of DOL induced by LiPF6. (B) Optical photographs of LE and GPE. (C) 1H NMR spectrum of PDXL. Photo credit: Feng-Quan Liu, Beijing Normal University. (D) Variation processes of molecular weight (blue dotted line) and ionic conductivity (red dotted line) during gelation process.

  • Fig. 2 Electrochemical tests and Li morphologies of Li|Li symmetrical batteries with GPE and LE.

    Curves of Li|GPE|Li (red lines) and Li|LE|Li (blue lines) symmetrical batteries at room temperature with the current densities of (A) 0.5 mA cm−2 for 1.0 mAh cm−2 and (B) 1.0 mA cm−2 for 1.0 mAh cm−2. (C) Surface morphology and (D) cross-sectional morphology of Li anode in GPE system after cycling at 1.0 mA cm−2. (E) Surface morphology and (F) cross-sectional morphology of Li anode in LE system after cycling at 1.0 mA cm−2.

  • Fig. 3 Schematic diagram, SEM, and optical morphologies of the GPE applied in the Li-S battery.

    (A) Schematic diagram of the in situ polymerization inside the battery system. Surface morphologies of (B) KB (Ketjen black)/S composite cathode and (C) separator before polymerization. Surface morphologies of (D) KB/S composite cathode and (E) separator after polymerization. (F) Permeation behavior of Li2S8 in LE (left) and GPE (right). Photo credit: Wen-Peng Wang, Institute of Chemistry, Chinese Academy of Sciences. (G) Optical photographs of separators harvested from the Li-S batteries with LE (left) and GPE (right) after 50 cycles at 0.5 C. Photo credit: Feng-Quan Liu, Beijing Normal University.

  • Fig. 4 Electrochemical performances of Li-S batteries with GPE and LE.

    Charge/discharge curves of Li-S batteries (A) with GPE and (B) with LE for the first three cycles at the rate of 0.5 C. The CV curves of Li-S batteries (C) with GPE and (D) with LE for the first three cycles at a scanning rate of 0.05 mV s−1. (E) Cycling performance and Coulombic efficiency of the batteries with GPE and LE.

  • Fig. 5 Electrochemical performances of LiFePO4|GPE|Li battery and LiFePO4|LE|Li battery.

    (A) Charge/discharge curves of LiFePO4|GPE|Li battery. (B) Cycling performance and Coulombic efficiency of LiFePO4|GPE|Li battery and LiFePO4|LE|Li battery.

  • Fig. 6 Electrochemical performances of NCM622|GPE|Li battery and NCM622|LE|Li battery.

    LSV curves of (A) LE and (C) GPE with the voltage range of 2.5 to 5.0 V at room temperature. Charge/discharge curves of (B) NCM622|LE|Li battery and (D) NCM622|GPE|Li battery with the voltage range of 2.8 to 4.3 V. (E) Cycling performance and Coulombic efficiency of NCM622|GPE|Li battery. (F) Optical images of LED lamps lighted by flexible NCM622|GPE|Li battery under various mechanical deformations. Photo credit: Wen-Peng Wang, Institute of Chemistry, Chinese Academy of Sciences.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/10/eaat5383/DC1

    Fig. S1. Contact angle measurement of the polymer precursor and LE on the different substrates.

    Fig. S2. GC-MS of mixed gases.

    Fig. S3. Thermogravimetric analysis and differential scanning calorimetry curves of LiPF6.

    Fig. S4. Effect of H2O content on polymerization.

    Fig. S5. Polymerization mechanism of DOL induced by LiPF6.

    Fig. S6. XPS spectra of LiPF6 and GPE.

    Fig. S7. 13C NMR spectrum of PDXL (deuterated chloroform as solvent).

    Fig. S8. FTIR spectrum of PDXL.

    Fig. S9. Characteristic changes of GPE during the whole polymerization progress.

    Fig. S10. EIS curves of the GPE with various DME content in the precursors.

    Fig. S11. Volatilization property of GPE and LE.

    Fig. S12. Thermal analysis of the PDXL and polyethylene oxide (PEO).

    Fig. S13. Electrochemical tests of the Li-Cu batteries with GPE and LE.

    Fig. S14. Cross-sectional SEM image of the as-prepared cathode and separator soaked with GPE.

    Fig. S15. EIS and anode SEM images of Li-S batteries with GPE and LE.

    Fig. S16. XPS of the Li anodes of the Li-S batteries with GPE and LE after 50 cycles at 0.5 C.

    Fig. S17. Self-discharge tests and soft-package Li-S battery.

    Fig. S18. Charge/discharge curves of LiFePO4|LE|Li battery.

    Fig. S19. Mechanical property of GPE with a special shape at room temperature.

    Table S1. Polymerization conversion rate of DOL in the electrolyte from monomer to polymer.

    Table S2. Ion conductivity of GPE with various DME content in the precursors.

    Movie S1. Contact angle measurement of polymer precursor and LE on cathode substrates.

  • Supplementary Materials

    The PDF file includes:

    • Fig. S1. Contact angle measurement of the polymer precursor and LE on the different substrates.
    • Fig. S2. GC-MS of mixed gases.
    • Fig. S3. Thermogravimetric analysis and differential scanning calorimetry curves of LiPF6.
    • Fig. S4. Effect of H2O content on polymerization.
    • Fig. S5. Polymerization mechanism of DOL induced by LiPF6.
    • Fig. S6. XPS spectra of LiPF6 and GPE.
    • Fig. S7. 13C NMR spectrum of PDXL (deuterated chloroform as solvent).
    • Fig. S8. FTIR spectrum of PDXL.
    • Fig. S9. Characteristic changes of GPE during the whole polymerization progress.
    • Fig. S10. EIS curves of the GPE with various DME content in the precursors.
    • Fig. S11. Volatilization property of GPE and LE.
    • Fig. S12. Thermal analysis of the PDXL and polyethylene oxide (PEO).
    • Fig. S13. Electrochemical tests of the Li-Cu batteries with GPE and LE.
    • Fig. S14. Cross-sectional SEM image of the as-prepared cathode and separator soaked with GPE.
    • Fig. S15. EIS and anode SEM images of Li-S batteries with GPE and LE.
    • Fig. S16. XPS of the Li anodes of the Li-S batteries with GPE and LE after 50 cycles at 0.5 C.
    • Fig. S17. Self-discharge tests and soft-package Li-S battery.
    • Fig. S18. Charge/discharge curves of LiFePO4|LE|Li battery.
    • Fig. S19. Mechanical property of GPE with a special shape at room temperature.
    • Table S1. Polymerization conversion rate of DOL in the electrolyte from monomer to polymer.
    • Table S2. Ion conductivity of GPE with various DME content in the precursors.

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    Other Supplementary Material for this manuscript includes the following:

    • Movie S1 (.mp4 format). Contact angle measurement of polymer precursor and LE on cathode substrates.

    Files in this Data Supplement:

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