Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in ..beta..-Li3PS4 Ceramic Electrolyte

Natalie Seitzman, Harvey Guthrey, Dana Kern, Mowafak Al-Jassim, Heather Platt, Svitlana Pylypenko

Research output: Contribution to journalArticlepeer-review

49 Scopus Citations


All-solid lithium batteries are an attractive next-generation technology that use ion-conducting solids such as β-Li3PS4 (LPS) to enable use of a lithium metal anode, which increases theoretical capacity and widens the stable voltage window over traditional lithium-ion systems. These ion-conductive solids also provide increased safety by replacing flammable liquid electrolytes. Although solid-state electrolytes are significantly more stable and dendrite-resistant than traditional liquid electrolytes, lithium anodes in all-solid systems may nevertheless grow dendrites under high stress or repeated cycling, leading to short circuits and premature battery breakdown. For this reason, we study the formation and propagation of Li metal features within solid electrolytes using synchrotron-based X-ray tomography with in-situ current-voltage cycling supported by our custom sample platform. Our results demonstrate the ability of this technique to delineate different layers of the Li/LPS/Li structure with spatial resolution approaching 1 μm. At this resolution, we are able to detect expansion of voids, especially in early stages of cycling. This expansion of voids is observed throughout the volume of the symmetric cells and visually resembles propagation of cracks resulting from interactions between the Li metal and pre-existing voids in the LPS electrolyte.

Original languageAmerican English
Pages (from-to)A3732-A3737
JournalJournal of the Electrochemical Society
Issue number16
StatePublished - 2018

Bibliographical note

Publisher Copyright:
© 2018 The Electrochemical Society.

NREL Publication Number

  • NREL/JA-5K00-71923


  • batteries
  • lithium dendrites
  • solid electrolytes
  • surface science
  • x-ray tomography


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