Visualizing plating-induced cracking in lithium-anode solid-electrolyte cells

Ziyang Ning, Dominic Spencer Jolly, Guanchen Li, Robin De Meyere, Shengda D. Pu, Yang Chen, Jitti Kasemchainan, Johannes Ihli, Chen Gong, Boyang Liu, Dominic L.R. Melvin, Anne Bonnin, Oxana Magdysyuk, Paul Adamson, Gareth O. Hartley, Charles W. Monroe, T. James Marrow, Peter G. Bruce

Research output: Contribution to journalArticlepeer-review

189 Citations (SciVal)

Abstract

Lithium dendrite (filament) propagation through ceramic electrolytes, leading to short circuits at high rates of charge, is one of the greatest barriers to realizing high-energy-density all-solid-state lithium-anode batteries. Utilizing in situ X-ray computed tomography coupled with spatially mapped X-ray diffraction, the propagation of cracks and the propagation of lithium dendrites through the solid electrolyte have been tracked in a Li/Li6PS5Cl/Li cell as a function of the charge passed. On plating, cracking initiates with spallation, conical ‘pothole’-like cracks that form in the ceramic electrolyte near the surface with the plated electrode. The spallations form predominantly at the lithium electrode edges where local fields are high. Transverse cracks then propagate from the spallations across the electrolyte from the plated to the stripped electrode. Lithium ingress drives the propagation of the spallation and transverse cracks by widening the crack from the rear; that is, the crack front propagates ahead of the Li. As a result, cracks traverse the entire electrolyte before the Li arrives at the other electrode, and therefore before a short circuit occurs.

Original languageEnglish
Pages (from-to)1121-1129
Number of pages10
JournalNature Materials
Volume20
Issue number8
Early online date22 Apr 2021
DOIs
Publication statusPublished - 31 Aug 2021

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

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