Research ArticleENERGY STORAGE

High–energy density nonaqueous all redox flow lithium battery enabled with a polymeric membrane

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Science Advances  27 Nov 2015:
Vol. 1, no. 10, e1500886
DOI: 10.1126/sciadv.1500886
  • Fig. 1 Concept of an RFLB full cell and a summary of the reported energy density of various aqueous and nonaqueous RFBs.

    (A) Schematic illustration of a redox flow lithium battery (RFLB) full cell. It has two separate tanks filled with porous LiFePO4 and TiO2 granules. Catholyte and anolyte are circulated through the materials in the tanks and to the cell during charging and discharging. (B) Photograph of an RFLB full cell used in this report. Electrolytes are circulated with two peristaltic pumps. (C) A plot summarizing various flow-type battery chemistries in terms of cell voltage, effective concentration of redox species (by considering the number of electrons involved in the reaction), and energy density.

  • Fig. 2 General properties of Nafion/PVDF membranes.

    (A) Impedance Nyquist plots of the NP11 membrane before and after testing in an RFLB full cell for 47 cycles. The inset also shows the photographs of an OHARA LICGC and NP11 membrane before and after cycling. (B and C) AFM phase image (B) and energy-dispersive x-ray spectroscopy (EDX) elemental mapping (C) of the as-prepared NP11 membrane.

  • Fig. 3 Working principle of the redox targeting reactions in cathodic and anodic tanks.

    (A) Cyclic voltammograms of the redox mediators and Li storage materials—LiFePO4 and TiO2. (B) A scheme compiling the chemical reactions between the redox mediators and materials in the tanks, as well as the electrochemical reactions of the mediators in the cell at different charging and discharging stages.

  • Fig. 4 Electrochemical performance of the RFLB full cell.

    (A) Typical voltage profiles of the RFLB full cell at different current densities. The inset shows a fraction of the GITT curve of the cell during the charging process at a current density of 0.05 mA cm−2. (B) Volumetric capacity retention and coulombic efficiency of the cell over cycling at different current densities.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/1/10/e1500886/DC1

    RFLB full cell performance with a lithiated Nafion 212 membrane

    Fig. S1. Voltage profiles of an RFLB full cell using the lithiated Nafion 212 membrane.

    Swelling and solvent uptake of lithiated Nafion 212 and NP11 membranes

    Table S1. Swelling and PC uptake of the lithiated Nafion 212 and NP11 membrane.

    Resistance of an RFLB with the NP11 membrane

    Fig. S2. Nyquist plots of the impedance of the NP11 membrane measured in an RFLB cell after different durations of electrolyte circulation.

    AFM phase image of a lithiated Nafion 212 membrane

    Fig. S3. AFM image of a lithiated Nafion 212 membrane for comparison.

    Permeability test of redox mediators across different membranes

    Fig. S4. Permeability study of the membranes.

    Morphological characterization of the NP11 membrane before and after cycling

    Fig. S5. Morphological features of the NP11 membrane.

    Areal resistance of Nafion and composite membranes

    Table S2. Comparison of the areal resistance, conductivity, and DL of different membranes.

    Cell performance of an RFLB full cell with the NP21 membrane

    Fig. S6. Cell performance of an RFLB with the NP21 membrane.

    Fig. S7. Nyquist plots of the impedance of a conductivity cell with different membranes.

    AFM image of the NP11 membrane after cycling in an RFLB full cell

    Fig. S8. AFM image of the NP11 membrane after cycling in an RFLB full cell.

    FTIR spectra of the NP11 membrane before and after cycling in an RFLB full cell

    Fig. S9. FTIR spectra of the NP11 membrane before and after cycling in an RFLB full cell.

    RFLB full cell performance with the NP11 membrane

    Fig. S10. Voltage profiles of the RFLB full cell.

  • Supplementary Materials

    This PDF file includes:

    • RFLB full cell performance with a lithiated Nafion 212 membrane
    • Fig. S1. Voltage profiles of an RFLB full cell using the lithiated Nafion 212 membrane.
    • Swelling and solvent uptake of lithiated Nafion 212 and NP11 membranes
    • Table S1. Swelling and PC uptake of the lithiated Nafion 212 and NP11 membrane.
    • Resistance of an RFLB with the NP11 membrane
    • Fig. S2. Nyquist plots of the impedance of the NP11 membrane measured in an RFLB cell after different durations of electrolyte circulation.
    • AFM phase image of a lithiated Nafion 212 membrane
    • Fig. S3. AFM image of a lithiated Nafion 212 membrane for comparison.
    • Permeability test of redox mediators across different membranes
    • Fig. S4. Permeability study of the membranes.
    • Morphological characterization of the NP11 membrane before and after cycling
    • Fig. S5. Morphological features of the NP11 membrane.
    • Areal resistance of Nafion and composite membranes
    • Table S2. Comparison of the areal resistance, conductivity, and DL of different membranes.
    • Cell performance of an RFLB full cell with the NP21 membrane
    • Fig. S6. Cell performance of an RFLB with the NP21 membrane.
    • Fig. S7. Nyquist plots of the impedance of a conductivity cell with different membranes.
    • AFM image of the NP11 membrane after cycling in an RFLB full cell
    • Fig. S8. AFM image of the NP11 membrane after cycling in an RFLB full cell.
    • FTIR spectra of the NP11 membrane before and after cycling in an RFLB full cell
    • Fig. S9. FTIR spectra of the NP11 membrane before and after cycling in an RFLB full cell.
    • RFLB full cell performance with the NP11 membrane
    • Fig. S10. Voltage profiles of the RFLB full cell.

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