Research ArticleMATERIALS SCIENCE

Stretchable batteries with gradient multilayer conductors

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Science Advances  26 Jul 2019:
Vol. 5, no. 7, eaaw1879
DOI: 10.1126/sciadv.aaw1879
  • Fig. 1 Schematic illustration of GAP multilayer conductors.

    Stratified assembly of stretchable nanocomposites with different concentrations of Au NPs in the elastic layer. The interface boundary of the layered structure is stratified by the sequential filtration of each AuPU composite suspension with different concentration gradients. The photographs show a GAP multilayer conductor under relaxed and strained conditions. (Photo credit: Woo-Jin Song, Pohang University of Science and Technology)

  • Fig. 2 Architecture-controlled GAP multilayer conductors.

    Schematic illustrations and representative cross-sectional SEM images with elemental mapping images of carbon and Au of (A) high-gradient (90/50/90 wt % AuPU) and (B) low-gradient (90/85/90 wt % AuPU) multilayer conductors with an increasing number of layers. Scale bars, 20 μm.

  • Fig. 3 Mechanical properties of GAP multilayer conductors.

    (A) Stress-strain curves for all GAP multilayer conductors. (B and C) Young’s modulus and rupture point of low and high GAP multilayer conductors. Finite element analysis of (directional) stress distribution in the (D) horizontal and (E) vertical directions for 5 L and 9 L low GAP conductors under 50% strain.

  • Fig. 4 Electrical properties of GAP multilayer conductors and small-angle x-ray scattering analysis for the percolation network of Au NPs in a PU matrix under strain.

    (A) Normalized resistance on the top surface of high and low GAP multilayer conductors of 3 L and 9 L under different strain conditions. (B) Calculation of vertical conductivity for low GAP conductors with increasing number of layers. (C) Change in vertical conductivity in 5 L and 9 L low GAP conductors under strain. (D) Schematic illustration of the experimental setup of in situ small-angle x-ray scattering (SAXS) measurement. (E) 2D SAXS patterns at selected uniaxial strains of 0, 50, and 100% for pure PU and 50 wt % AuPU nanocomposite films, and schematic illustrations summarizing the behavior of Au NPs (yellow spheres) in the matrix and changes in the electrical pathway (red lines) under strain determined by SAXS analysis. (F) Calculated Herman’s orientation factor, f, under strain for a single layer of PU and 50 wt % AuPU.

  • Fig. 5 Electrochemical performance of stretchable aqueous rechargeable lithium-ion battery using a GAP multilayer conductor as a current collector.

    (A) CV profiles of the GAP anode (PI/CNT) and GAP cathode (LMO/CNT) at various current densities in three electrode systems in a 1 M Li2SO4 electrolyte with a Pt electrode and an Ag/AgCl electrode as the counter and reference electrodes, respectively. (B and C) Galvanostatic charge-discharge curves of the GAP cathode and GAP anode, respectively. (D) Cycling performance of the full battery at a current density of 0.5 A g−1 between 0.0 and 2.2 V in 1 M Li2SO4 for 1000 cycles. (E) Schematic illustration of the stretchable aqueous rechargeable lithium-ion battery fabricated using the GAP anode and cathode with a coplanar layout. (F) Cycle performance of the stretchable full cell at a current density of 0.5 A g−1 under various strains of 0 to 30% for 100 cycles. (G) Capacity retention as a function of cycle at a current density of 0.5 A g−1. The stretchable battery was pulled 20 times at a strain of 30% for each group of 20 electrochemical cycles. (H) Photographs of an LED bulb operated using stretchable aqueous lithium-ion battery under strains of 0 and 30%. (Photo credit: Woo-Jin Song, Pohang University of Science and Technology)

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/5/7/eaaw1879/DC1

    Fig. S1. Schematic illustration and TEM image with a corresponding size distribution histogram of citrate-stabilized Au NPs.

    Fig. S2. Characterization of the single layer.

    Fig. S3. Resistance and conductivity.

    Fig. S4. The specific contents of the Au NPs in the high- and low-gradient multilayer conductors.

    Fig. S5. SEM of the 9 L high GAP conductor under strain.

    Fig. S6. Cross-sectional SEM of the 9 L high GAP conductor under a strain of 100%.

    Fig. S7. High-resolution SEM.

    Fig. S8. Finite element analysis of (directional) stress distribution.

    Fig. S9. Change of resistance on the top surface of 9 L high GAP multilayer conductors under dynamic stretching between 0% strain (orange region) and different uniaxial strains (green region) during 1000 cycles.

    Fig. S10. In situ SAXS analysis.

    Fig. S11. Characterization of anode materials.

    Fig. S12. Characterization of cathode materials.

    Fig. S13. Top-view SEM images of active materials.

    Fig. S14. Top-view SEM of active materials on a 9 L high GAP conductor under strain.

    Fig. S15. Half-cell test of the cathode and anode.

    Fig. S16. Top-view SEM images.

    Fig. S17. Galvanostatic charge-discharge curves of the full cell at various current densities.

    Fig. S18. Voltage curves of the stretchable full cell as a function of time at various current densities.

    Fig. S19. Fatigue test of the stretchable battery under 50% strain over 100 cycles.

    Fig. S20. Voltage curves of series stretchable full battery in the voltage range from 0 to 4.0 V as a function of time.

    Movie S1. LED bulb operated using a stretchable aqueous lithium-ion battery.

  • Supplementary Materials

    The PDF file includes:

    • Fig. S1. Schematic illustration and TEM image with a corresponding size distribution histogram of citrate-stabilized Au NPs.
    • Fig. S2. Characterization of the single layer.
    • Fig. S3. Resistance and conductivity.
    • Fig. S4. The specific contents of the Au NPs in the high- and low-gradient multilayer conductors.
    • Fig. S5. SEM of the 9 L high GAP conductor under strain.
    • Fig. S6. Cross-sectional SEM of the 9 L high GAP conductor under a strain of 100%.
    • Fig. S7. High-resolution SEM.
    • Fig. S8. Finite element analysis of (directional) stress distribution.
    • Fig. S9. Change of resistance on the top surface of 9 L high GAP multilayer conductors under dynamic stretching between 0% strain (orange region) and different uniaxial strains (green region) during 1000 cycles.
    • Fig. S10. In situ SAXS analysis.
    • Fig. S11. Characterization of anode materials.
    • Fig. S12. Characterization of cathode materials.
    • Fig. S13. Top-view SEM images of active materials.
    • Fig. S14. Top-view SEM of active materials on a 9 L high GAP conductor under strain.
    • Fig. S15. Half-cell test of the cathode and anode.
    • Fig. S16. Top-view SEM images.
    • Fig. S17. Galvanostatic charge-discharge curves of the full cell at various current densities.
    • Fig. S18. Voltage curves of the stretchable full cell as a function of time at various current densities.
    • Fig. S19. Fatigue test of the stretchable battery under 50% strain over 100 cycles.
    • Fig. S20. Voltage curves of series stretchable full battery in the voltage range from 0 to 4.0 V as a function of time.

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    Other Supplementary Material for this manuscript includes the following:

    • Movie S1 (.avi format). LED bulb operated using a stretchable aqueous lithium-ion battery.

    Files in this Data Supplement:

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