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 language | English |
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Pages (from-to) | 1121-1129 |
Number of pages | 10 |
Journal | Nature Materials |
Volume | 20 |
Issue number | 8 |
Early online date | 22 Apr 2021 |
DOIs | |
Publication status | Published - 31 Aug 2021 |
Bibliographical note
Funding Information:P.G.B. is indebted to the Faraday Institution All-Solid-State Batteries with Li and Na Anodes (FIRG007, FIRG008), as well as the Engineering and Physical Sciences Research Council, Enabling Next Generation Lithium Batteries (EP/M009521/1), the University of Oxford experimental equipment upgrade (EP/M02833X/1) and the Henry Royce Institute for Advanced Materials (EP/R0066X/1, EP/S019367/1, EP/R010145/1) for financial support. G.L. and C.W.M. acknowledge the Faraday Institution Multiscale Modelling (FIRG003) and the UK Industrial Strategy Challenge Fund: Materials Research Hub for Energy Conversion, Capture, and Storage, under grant EP/R023581/1, for financial support. J.I. is supported by the Swiss National Science Foundation (no. PZ00P2_179886). We thank Paul Scherrer Institut, Villigen, Switerland, and Diamond Light Source, Harwell, United Kingdom, for provision of synchrotron radiation beam time (experiment no. 20182142) at the TOMCAT beamline X02DA of the Swiss Light Source, and beam time (experiment no. EE20795-1) at the I12 beamline of the Diamond Light Source. We acknowledge technical and experimental support at the TOMCAT by A. Bonnin and J. Ihli, and at the I12 by O. Magdysyuk.
Data availability:
Supporting research data have been deposited in the Oxford Research Archive and are available at https://doi.org/10.5287/bodleian:9Rn6n6o15.
ASJC Scopus subject areas
- General Chemistry
- General Materials Science
- Condensed Matter Physics
- Mechanics of Materials
- Mechanical Engineering