Research ArticleMATERIALS SCIENCE

Printable, high-performance solid-state electrolyte films

See allHide authors and affiliations

Science Advances  18 Nov 2020:
Vol. 6, no. 47, eabc8641
DOI: 10.1126/sciadv.abc8641
  • Fig. 1 PRH process for film synthesis.

    (A) Schematic of the film printing technique, which uses a ceramic precursor ink and a rapid sintering process that heats the material to high temperature (1500°C) within ~3 s. (B) The sintered LLZTO garnet film on a single-crystal MgO substrate. (C) The corresponding profilometry curve of the sintered film. Photo credit: Weiwei Ping, University of Maryland, College Park.

  • Fig. 2 Optimization of ceramic film printing and sintering conditions.

    (A) SSE precursor ink prepared by dispersing the mixed oxide precursors (Li2CO3, La2O3, ZrO2, and Ta2O5) in ethanol. (B) The SSE ink shows good fluidity. (C) Printing the garnet precursor ink by spray coating through a mask. (D) Printing the SSE precursor ink by the doctor blade method. (E) The printed SSE film is scalable and flexible. (F to H) Schematic and cross-sectional morphology of LLZTO garnet films sintered at different temperatures and times, in which an adequate sintering temperature with appropriate sintering time is necessary to acquire a dense garnet film with limited Li loss and uniform grain size distribution. XRD patterns of LLZTO films sintered at temperatures ranging from (I) 800° to 1300°C and hold times ranging from 1 to 180 s and at (J) 1400° to 1700°C and hold times ranging from 1 to 10 s. a.u., arbitrary units. Photo credit: Weiwei Ping, University of Maryland, College Park.

  • Fig. 3 Performance of PRH-sintered LLZTO film.

    (A) Cross-sectional SEM image and (B) EDS mapping of the sintered LLZTO film on an Al2O3 substrate. (C) Surface morphology of the sintered LLZTO film on the Al2O3 substrate. (D) Statistics of the grain size distribution of the sintered LLZTO film. (E) Activation energy of the PRH-sintered LLZTO film, fitted to an Arrhenius relationship. (F) Voltage and current profiles of the symmetric Li/LLZTO/Li cell with in-plane Li electrodes for critical current density test. (G) Comparison of Li loss in films sintered by PRH and conventional methods. (H) Comparison of the ionic conductivity at room temperature of SSE films synthesized by the PRH method and other reported techniques (2, 8, 9, 11, 3541).

  • Fig. 4 Other SSE films sintered by PRH.

    (A) The printing inks of LLTO, LATP, β-Al2O3, and LiBO2-LLZTO precursors. (B) Left: The cross-sectional morphology and elemental mapping results of the PRH-sintered LLTO, LATP, β-Al2O3 films. Right: Schematic of the volatile element loss comparison between PRH and conventional sintering methods. (C) Left: The cross-sectional morphology and mapping results of the PRH-sintered LiBO2-LLZTO film. Right: Schematic of the side reaction control comparison between PRH and conventional methods. Photo credit: Weiwei Ping, University of Maryland, College Park.

  • Fig. 5 All-solid-state battery LiBO2-LiCoO2/LLZTO/Li sintered by PRH.

    (A) The printing and sintering process of the PRH-fabricated solid-state battery. (B) Cross-sectional SEM image and (C) EDS mapping of the PRH-sintered LiCoO2 cathode on the LLZTO surface. (D) Cross-sectional and (E) magnified SEM images of the LiBO2-LiCoO2/LLZTO interface. (F) EIS spectra of the all-solid-state battery (LiBO2-LiCoO2/LLZTO/Li) before cycling and after the 450th cycle. (G) Voltage profiles of the in situ fabricated all-solid-state battery at different current densities. (H) Cycling performance and Coulombic efficiency of the LiBO2-LiCoO2/LLZTO/Li all-solid-state battery at 60°C.

Supplementary Materials

  • Supplementary Materials

    Printable, high-performance solid-state electrolyte films

    Weiwei Ping, Chengwei Wang, Ruiliu Wang, Qi Dong, Zhiwei Lin, Alexandra H. Brozena, Jiaqi Dai, Jian Luo, Liangbing Hu

    Download Supplement

    This PDF file includes:

    • Figs. S1 to S21

    Files in this Data Supplement:

Stay Connected to Science Advances

Navigate This Article