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A low ride on processing temperature for fast lithium conduction in garnet solid-state battery films

Nature Energy volume 4, pages 475–483 (2019)Cite this article

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Abstract

A critical parameter for the large-scale integration of solid-state batteries is to establish processing strategies to assemble battery materials at the lowest processing temperature possible while keeping lithium conduction up. Despite extensive research efforts, integrating ceramic film electrolytes while keeping a high lithium concentration and conduction at a low processing temperature remains challenging. Here, we report an alternative ceramic processing strategy through the evolution of multilayers establishing lithium reservoirs directly in lithium–garnet films that allow for lithiated and fast-conducting cubic solid-state battery electrolytes at unusually low processing temperatures. A lithium–garnet film processed via the multilayer processing approach exhibited the fastest ionic conductivity of 2.9 ± 0.05 × 10−5 S cm−1 (at room temperature) and the desired cubic phase, but was stabilized at a processing temperature lowered by 400 °C. This method enables future solid-state battery architectures with more room for cathode volumes by design, and reduces the processing temperature.

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Fig. 1: Experimental approach for thin-film deposition of Li–garnet.
Fig. 2: Merging of the multilayered structure.
Fig. 3: Negative-ion TOF-SIMS spectrum of a thin film.
Fig. 4: Ex situ phase evolution.
Fig. 5: Raman spectra of selected thin films deposited by PLD under optimal conditions using three different approaches.
Fig. 6: Ionic transport properties in thin-film Li–garnet.
Fig. 7: Processing temperature dependence in Li–garnets.

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

The authors thank the Competence Center Energy and Mobility and Swiss Electrics for funding the project ‘All solid state Li-ion batteries based on new ceramic Li-ion electrolytes’ (proposal 911). J.L.M.R. thanks Lincoln Laboratory project ACC 697 (2018) and the Thomas Lord Foundation for financial support.

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Author notes

  1. Michal Struzik

    Present address: Faculty of Physics, Warsaw University of Technology, Warsaw, Poland

  2. Iñigo Garbayo

    Present address: CIC Energigune, Parque Tecnológico de Álava, Miñano, Spain

Authors and Affiliations

  1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Reto Pfenninger, Michal Struzik & Jennifer L. M. Rupp

  2. Electrochemical Materials, Swiss Federal Institute of Technology, Zurich, Switzerland

    Reto Pfenninger, Michal Struzik, Iñigo Garbayo & Jennifer L. M. Rupp

  3. Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland

    Evelyn Stilp

  4. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA

    Jennifer L. M. Rupp

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Contributions

R.P., M.S., I.G. and E.S. carried out the experiments. R.P., M.S., I.G., E.S. and J.L.M.R. performed the analysis and discussed the data. R.P. and J.L.M.R. wrote the manuscript with help from all of the co-authors.

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Correspondence to Jennifer L. M. Rupp.

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Supplementary notes 1 and 2, Supplementary Figs. 1–7, Supplementary discussion, Supplementary references

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Pfenninger, R., Struzik, M., Garbayo, I. et al. A low ride on processing temperature for fast lithium conduction in garnet solid-state battery films. Nat Energy 4, 475–483 (2019). https://doi.org/10.1038/s41560-019-0384-4

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