High-power all-solid-state batteries using sulfide superionic conductors

Abstract

Compared with lithium-ion batteries with liquid electrolytes, all-solid-state batteries offer an attractive option owing to their potential in improving the safety and achieving both high power and high energy densities. Despite extensive research efforts, the development of all-solid-state batteries still falls short of expectation largely because of the lack of suitable candidate materials for the electrolyte required for practical applications. Here we report lithium superionic conductors with an exceptionally high conductivity (25 mS cm−1 for Li9.54Si1.74P1.44S11.7Cl0.3), as well as high stability ( 0 V versus Li metal for Li9.6P3S12). A fabricated all-solid-state cell based on this lithium conductor is found to have very small internal resistance, especially at 100 C. The cell possesses high specific power that is superior to that of conventional cells with liquid electrolytes. Stable cycling with a high current density of 18 C (charging/discharging in just three minutes; where C is the C-rate) is also demonstrated.

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Figure 1: X-ray diffraction patterns of the LGPS family.
Figure 2: Ionic conductivity and crystal structure of Li9.54Si1.74P1.44S11.7Cl0.3.
Figure 3: Electrochemical stability of the LGPS family.
Figure 4: Performance of the all-solid-state cells.
Figure 5: Chronoamperometric behaviours of the all-solid-state and lithium-ion cells.
Figure 6: The Ragone plot.

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Acknowledgements

The authors thank T. Yabutani, R. Saito and K. Mukoyama for their support in the preparation of the all-solid-state and lithium-ion cells. They also thank H. Hirokawa for his support in the synthesis of Li9.6P3S12. This study was supported by the Post-LiEAD project of the New Energy and Industry Technology Development Organization (NEDO), Japan. The synchrotron radiation experiments were carried out as projects approved by the Japan Synchrotron Radiation Institute (JASRI) (proposal No. 2014A1408 and 2014A1763). The neutron radiation experiments were performed at the Japan Proton Accelerator Research Complex (J-PARC) (proposal No. 2014AM1004, 2014BM0006 and 2014BM0012).

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Contributions

Y.K. and S.H. designed and conducted the experimental work. Y.K., S.H., T.S., K.S., M.H. and R.K. analysed the electrochemical data. S.H., A.M. and M.Y. measured the synchrotron X-ray and neutron diffraction of superionic conductors. Y.K., S.H., M.Y. and R.K. analysed the crystal structure. Y.K., S.H. and R.K. wrote the manuscript. H.I. and R.K. directed this work.

Corresponding authors

Correspondence to Yuki Kato or Ryoji Kanno.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Figures 1–12, Supplementary Table 1–6, Supplementary Methods and Supplementary References. (PDF 2379 kb)

Supplementary Video 1

Description of the bi-polar stacking cell system. (MP4 47865 kb)

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Kato, Y., Hori, S., Saito, T. et al. High-power all-solid-state batteries using sulfide superionic conductors. Nat Energy 1, 16030 (2016). https://doi.org/10.1038/nenergy.2016.30

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