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

doi:10.1038/s41563-021-00967-8

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

Department of Mechanical Engineering

Research output: Contribution to journal › Article › peer-review

312 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 language	English
Pages (from-to)	1121-1129
Number of pages	10
Journal	Nature Materials
Volume	20
Issue number	8
Early online date	22 Apr 2021
DOIs	https://doi.org/10.1038/s41563-021-00967-8
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.

Funding

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.

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/s41563-021-00967-8

https://ora.ox.ac.uk/objects/uuid:f32ca761-2a41-4609-a25c-5b2071e247f4

Cite this

Ning, Z., Jolly, D. S., Li, G., De Meyere, R., Pu, S. D., Chen, Y., Kasemchainan, J., Ihli, J., Gong, C., Liu, B., Melvin, D. L. R., Bonnin, A., Magdysyuk, O., Adamson, P., Hartley, G. O., Monroe, C. W., Marrow, T. J., & Bruce, P. G. (2021). Visualizing plating-induced cracking in lithium-anode solid-electrolyte cells. Nature Materials, 20(8), 1121-1129. https://doi.org/10.1038/s41563-021-00967-8

Ning, Z, Jolly, DS, Li, G, De Meyere, R, Pu, SD, Chen, Y, Kasemchainan, J, Ihli, J, Gong, C, Liu, B, Melvin, DLR, Bonnin, A, Magdysyuk, O, Adamson, P, Hartley, GO, Monroe, CW, Marrow, TJ & Bruce, PG 2021, 'Visualizing plating-induced cracking in lithium-anode solid-electrolyte cells', Nature Materials, vol. 20, no. 8, pp. 1121-1129. https://doi.org/10.1038/s41563-021-00967-8

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title = "Visualizing plating-induced cracking in lithium-anode solid-electrolyte cells",

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 {\textquoteleft}pothole{\textquoteright}-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.",

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

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.",

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AU - Ning, Ziyang

AU - Jolly, Dominic Spencer

AU - Li, Guanchen

AU - De Meyere, Robin

AU - Pu, Shengda D.

AU - Chen, Yang

AU - Kasemchainan, Jitti

AU - Ihli, Johannes

AU - Gong, Chen

AU - Liu, Boyang

AU - Melvin, Dominic L.R.

AU - Bonnin, Anne

AU - Magdysyuk, Oxana

AU - Adamson, Paul

AU - Hartley, Gareth O.

AU - Monroe, Charles W.

AU - Marrow, T. James

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N2 - 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.

AB - 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.

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

Abstract

Bibliographical note

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