4.8 Article

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

Journal

NATURE MATERIALS
Volume 20, Issue 8, Pages 1121-+

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41563-021-00967-8

Keywords

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Funding

  1. Faraday Institution All-Solid-State Batteries with Li and Na Anodes [FIRG007, FIRG008]
  2. Engineering and Physical Sciences Research Council
  3. Enabling Next Generation Lithium Batteries [EP/M009521/1]
  4. University of Oxford experimental equipment upgrade [EP/M02833X/1]
  5. Henry Royce Institute for Advanced Materials [EP/R0066X/1, EP/S019367/1, EP/R010145/1]
  6. Faraday Institution Multiscale Modelling [FIRG003]
  7. UK Industrial Strategy Challenge Fund: Materials Research Hub for Energy Conversion, Capture, and Storage [EP/R023581/1]
  8. Swiss National Science Foundation [PZ00P2_179886]
  9. Swiss National Science Foundation (SNF) [PZ00P2_179886] Funding Source: Swiss National Science Foundation (SNF)
  10. EPSRC [EP/M009521/1, EP/R023581/1, EP/M02833X/1] Funding Source: UKRI

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The propagation of lithium dendrites and cracks through ceramic electrolytes can lead to short circuits in batteries. The cracks initiate near the surface of the lithium electrode and propagate transversely across the electrolyte, driven by lithium ingress.
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. Lithium dendrite propagation through ceramic electrolytes can prevent the realization of high-energy-density all-solid-state lithium-anode batteries. The propagation of cracks and lithium dendrites through a solid electrolyte has now been tracked as a function of charge.

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