Research ArticleELECTROCHEMISTRY

Solid electrolyte interphases for high-energy aqueous aluminum electrochemical cells

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Science Advances  30 Nov 2018:
Vol. 4, no. 11, eaau8131
DOI: 10.1126/sciadv.aau8131
  • Fig. 1 Surface characterization of metal Al before (named as Al) and after treatment of AlCl3-IL electrolyte (named as TAl).

    (A) ATR-FTIR spectra of Al and TAl foil. XPS spectra of (B) Al2p, (C) Cl2p, and (D) N1s on the surface of Al foil (red line) and TAl foil (blue line). a.u., arbitrary units. SEM images of the surface of (E) Al foil and (F) TAl foil. The insets of (E) and (F) are digital photos of Al foil and TAl foil. (G) Cross-sectional SEM image of a TAl foil and corresponding EDX mapping of Al, Cl, and N.

  • Fig. 2 Electrochemical studies of aqueous electrolytes in Al batteries.

    (A) dc ionic conductivity of aqueous Al2(SO4)3 electrolyte and Al(CF3SO3)3 electrolytes with varying different concentrations as a function of temperature. (B) Electrochemical impedance spectroscopy (EIS) of symmetric Al batteries using different Al anodes and electrolytes. (C) Symmetric Al battery tests using Al and TAl coupled with different electrolytes. The current density is 0.2 mA cm−2. Each cycle contains the discharge process for 1 hour and the charge process for 1 hour, separately.

  • Fig. 3 Electrochemical performance of aqueous rechargeable Al batteries using α-MnO2 as the cathode.

    (A) Galvanostatic discharge/charge curves of aqueous Al batteries at a current density of 100 mA/g (MnO2) using TAl and electrolyte of 2 m Al(CF3SO3)3 in H2O. (B) CV diagram at scanning rates of 0.05, 0.10. 0.15, 0.20, 0.25, 0.30, and 0.35 mV/s. The inset is the linear fit of the square root of the scan rate and the peak current. (C) Cycling performance of aqueous Al batteries using Al or TAl and electrolyte of 2 m or 1 m Al(CF3SO3)3. (D) Rate performance at different current densities using TAl and 2 m Al(CF3SO3)3.

  • Fig. 4 Reaction mechanism of Al with α-MnO2 in aqueous electrolyte.

    (A) XRD patterns of MnO2 cathodes at fully discharged and charged states after different numbers of cycle. (B) Al/Mn ratio by SEM-EDX analysis of cathode after the first discharge and charge (washed or unwashed; include or subtract Al from electrolyte). (C) High-resolution TEM image and (D) corresponding enlarged view of pristine MnO2 cathode. The inset in (D) is the fast Fourier transform (FFT) of the image. (E) High-resolution TEM image, (F) FFT pattern, and (G) corresponding enlarged part of discharged MnO2 cathode. (H) Annular dark-field scanning transmission electron microscope (STEM) image and corresponding EELS mapping of fully discharged MnO2 cathode nanorod. (I) The two Mn valence states present were likely MnO2 and Mn3O4, as determined by multivariate curve resolution analysis of the Mn L2,3 edge.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/11/eaau8131/DC1

    Fig. S1. The SEM-EDX mapping spectra on the top view of TAL.

    Fig. S2. Rate performance of symmetric Al batteries using TAl and electrolyte of 1 m Al(CF3SO3)3 in water.

    Fig. S3. Symmetric Al battery performance using Al or TAl coupled with organic electrolyte.

    Fig. S4. The CV diagrams of Al-carbon fiber paper batteries.

    Fig. S5. ATR-FTIR spectra of different electrolytes.

    Fig. S6. Cross-sectional SEM image of TAl anode and corresponding EDX mapping after cycling in symmetric batteries.

    Fig. S7. SEM characterizations of MnO2 nanorod.

    Fig. S8. Galvanostatic discharge/charge curves of aqueous Al batteries using common Al anode.

    Fig. S9. Electrochemical properties of Al-MnO2 batteries using TAl anode–, Al(CF3SO3)3-, and Al2(SO4)3-based aqueous electrolyte.

    Fig. S10. GITT profiles of Al-MnO2 batteries.

    Fig. S11. Cycling performance comparisons with or without Mn(CF3SO3)2 addition at current density of 200 mA/g.

    Fig. S12. Galvanostatic discharge/charge curves at different current densities.

    Fig. S13. XRD patterns of MnO2 electrodes under different situations.

    Fig. S14. SEM images of MnO2 electrode.

    Fig. S15. SEM images and selected positions for EDX studies.

    Fig. S16. TEM images of MnO2 electrodes.

    Fig. S17. XPS Mn2p3/2 spectra of pristine MnO2, fully discharged MnO2 cathode, and fully charged MnO2 cathode.

    Table S1. EDX analysis of points in fig. S15.

    References (3236)

  • Supplementary Materials

    This PDF file includes:

    • Fig. S1. The SEM-EDX mapping spectra on the top view of TAL.
    • Fig. S2. Rate performance of symmetric Al batteries using TAl and electrolyte of 1 m Al(CF3SO3)3 in water.
    • Fig. S3. Symmetric Al battery performance using Al or TAl coupled with organic electrolyte.
    • Fig. S4. The CV diagrams of Al-carbon fiber paper batteries.
    • Fig. S5. ATR-FTIR spectra of different electrolytes.
    • Fig. S6. Cross-sectional SEM image of TAl anode and corresponding EDX mapping after cycling in symmetric batteries.
    • Fig. S7. SEM characterizations of MnO2 nanorod.
    • Fig. S8. Galvanostatic discharge/charge curves of aqueous Al batteries using common Al anode.
    • Fig. S9. Electrochemical properties of Al-MnO2 batteries using TAl anode–, Al(CF3SO3)3-, and Al2(SO4)3-based aqueous electrolyte.
    • Fig. S10. GITT profiles of Al-MnO2 batteries.
    • Fig. S11. Cycling performance comparisons with or without Mn(CF3SO3)2 addition at current density of 200 mA/g.
    • Fig. S12. Galvanostatic discharge/charge curves at different current densities.
    • Fig. S13. XRD patterns of MnO2 electrodes under different situations.
    • Fig. S14. SEM images of MnO2 electrode.
    • Fig. S15. SEM images and selected positions for EDX studies.
    • Fig. S16. TEM images of MnO2 electrodes.
    • Fig. S17. XPS Mn2p3/2 spectra of pristine MnO2, fully discharged MnO2 cathode, and fully charged MnO2 cathode.
    • Table S1. EDX analysis of points in fig. S15.
    • References (3236)

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