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Influence of temperature and ASR on the critical current density in lithium-metal–ceramic cells


We show a systematic correlation between temperature, critical current density (CCD), and ASR. The ASR declines while the CCD increases with temperature. The behavior is consistent with a void nucleation model for cell failure. Void nucleation is driven by the cell voltage: a lower ASR reduces the voltage which helps to raise the critical current density. The voids are postulated to be precipitated by local concentrations of electrochemical currents which pull lithium into the electrolyte leaving behind a void in the lithium layer across from the interface. We also report on a possible method for reducing the non-uniformity of current flow across the interface by introducing a layer of silver at the interface. It has the effect of increasing the CCD to 3.5 mA cm−2 at elevated temperature.

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  1. 1.

    A. Sharafi, H.M. Meyer, J. Nanda, J. Wolfenstine, J. Sakamoto, Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density. J. Power Sources 302, 135–139 (2016).

    CAS  Article  Google Scholar 

  2. 2.

    Y. Ren, Y. Shen, Y. Lin, C.-W. Nan, Direct observation of lithium dendrites inside garnet-type lithium-ion solid electrolyte. Electrochem. Commun. 57, 27–30 (2015).

    CAS  Article  Google Scholar 

  3. 3.

    A. Badran, T. Clemenceau, N. Andriamady, D. Marshall, R. Raj, Current constriction of Li-ion transport across lithium metal–ceramic electrolyte interface: imaged with X-ray Tomography. MRS Commun. (2021).

    Article  Google Scholar 

  4. 4.

    M. Wang, J.B. Wolfenstine, J. Sakamoto, Temperature dependent flux balance of the Li/Li7La3Zr2O12 interface. Electrochim. Acta 296, 842–847 (2019).

    CAS  Article  Google Scholar 

  5. 5.

    T. Krauskopf, B. Mogwitz, C. Rosenbach, W.G. Zeier, J. Janek, Diffusion limitation of lithium metal and Li–Mg alloy anodes on LLZO type solid electrolytes as a function of temperature and pressure. Adv. Energy Mater. 9, 1902568 (2019).

    CAS  Article  Google Scholar 

  6. 6.

    R. Raj, Stack pressure and critical current density in Li-metal cells: the role of mechanical deformation. Acta Materialia, in press (2021)

  7. 7.

    R. Raj, Nucleation of voids at Li-metal ceramic-electrolyte interfaces, in review (2021)

  8. 8.

    R. Raj, M.F. Ashby, Intergranular fracture at elevated temperature. Acta Metall. 23, 653–666 (1975).

    Article  Google Scholar 

  9. 9.

    L. Vitos, A.V. Ruban, H.L. Skriver, J. Kollár, The surface energy of metals. Surf. Sci. 411, 186–202 (1998).

    CAS  Article  Google Scholar 

  10. 10.

    G. Kiniger, V. Sglavo, S.K. Jha, R. Raj, Flash-induced spreading of metals on zirconia. Scripta Mater. 176, 73–77 (2020).

    CAS  Article  Google Scholar 

  11. 11.

    T. Clemenceau, N. Andriamady, P.M.K. Kumar, A. Badran, V. Avila, K. Dahl, M. Hopkins, X. Vendrell, D. Marshall, R. Raj, Flash sintering of Li-ion conducting ceramic in a few seconds at 850°C. Scripta Mater. 172, 1–5 (2019).

    CAS  Article  Google Scholar 

  12. 12.

    M. Cologna, B. Rashkova, R. Raj, Flash sintering of nanograin zirconia in < 5 s at 850°C: rapid communications of the American Ceramic Society. J. Am. Ceram. Soc. 93, 3556–3559 (2010).

    CAS  Article  Google Scholar 

  13. 13.

    V. Avila, R. Raj, Reactive flash sintering of powders of four constituents into a single phase of a complex oxide in a few seconds below 700°C. J. Am. Ceram. Soc. 102, 6443–6448 (2019).

    CAS  Article  Google Scholar 

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This research was supported by a project from ARPA-E award Number DE-AR0000777.

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Correspondence to Rishi Raj.

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On behalf of all authors, the corresponding author states that there is no conflict of interest. We do need to inform that a non-provisional patent based on the work on silver interlayer is currently being examined at the US Patent and Trademark Office.

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Clemenceau, T., Andriamady, N. & Raj, R. Influence of temperature and ASR on the critical current density in lithium-metal–ceramic cells. MRS Communications 11, 483–488 (2021).

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  • Ceramic
  • Sintering
  • Li
  • X-ray tomography
  • Interface