High plating currents without dendrites at the interface between a lithium anode and solid electrolyte

Dominic L. R. Melvin, Marco Siniscalchi, Dominic Spencer-Jolly, Bingkun Hu, Ziyang Ning, Shengming Zhang, Junfu Bu, Shashidhara Marathe, Anne Bonnin, Johannes Ihli, Gregory J. Rees, Patrick S. Grant, Charles W. Monroe, T. James Marrow, Guanchen Li () and Peter G. Bruce ()
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Dominic L. R. Melvin: University of Oxford
Marco Siniscalchi: University of Oxford
Dominic Spencer-Jolly: University of Oxford
Bingkun Hu: University of Oxford
Ziyang Ning: University of Oxford
Shengming Zhang: University of Oxford
Junfu Bu: University of Oxford
Shashidhara Marathe: Harwell Campus
Anne Bonnin: Paul Scherrer Institut
Johannes Ihli: University of Oxford
Gregory J. Rees: University of Oxford
Patrick S. Grant: University of Oxford
Charles W. Monroe: University of Oxford
T. James Marrow: University of Oxford
Guanchen Li: University of Glasgow
Peter G. Bruce: University of Oxford

Nature Energy, 2025, vol. 10, issue 10, 1205-1214

Abstract: Abstract Avoiding lithium dendrites at the lithium/ceramic electrolyte interface and, as a result, avoiding cell short circuit when plating at practical current densities remains a significant challenge for all-solid-state batteries. Typically, values are limited to around 1 mA cm−2, even, for example, for garnets with a relative density of >99%. It is not obvious that simply densifying ceramic electrolytes will deliver high plating currents. Here we show that plating currents of 9 mA cm−2 can be achieved without dendrite formation, by densifying argyrodite, Li6PS5Cl, to 99%. Changes in the microstructure of Li6PS5Cl on densification from 83 to 99% were determined by focused ion beam-scanning electron microscopy tomography and used to calculate their effect on the critical current density (CCD). Modelling shows that not all changes in microstructure with densification act to increase CCD. Whereas smaller pores and shorter cracks increase CCD, lower pore population and narrower cracks act to decrease CCD. Calculations show that the former changes dominate over the latter, predicating an overall increase in CCD, as observed experimentally.

Date: 2025
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DOI: 10.1038/s41560-025-01847-0

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