Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in β-Li 3 PS 4 Ceramic Electrolyte
Abstract
All-solid lithium batteries are an attractive next-generation technology that use ion-conducting solids such as ..beta..-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 um. 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.
- Authors:
-
- Colorado School of Mines, Golden, CO (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Solid Power, Inc. Louisville, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1492515
- Report Number(s):
- NREL/JA-5K00-71923
Journal ID: ISSN 0013-4651
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 165; Journal Issue: 16; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 30 DIRECT ENERGY CONVERSION; batteries; surface science; lithium dendrites; solid electrolytes; x-ray tomography
Citation Formats
Seitzman, Natalie, Guthrey, Harvey, Sulas, Dana B., Platt, Heather A. S., Al-Jassim, Mowafak, and Pylypenko, Svitlana. Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in β-Li 3 PS 4 Ceramic Electrolyte. United States: N. p., 2018.
Web. doi:10.1149/2.0301816jes.
Seitzman, Natalie, Guthrey, Harvey, Sulas, Dana B., Platt, Heather A. S., Al-Jassim, Mowafak, & Pylypenko, Svitlana. Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in β-Li 3 PS 4 Ceramic Electrolyte. United States. https://doi.org/10.1149/2.0301816jes
Seitzman, Natalie, Guthrey, Harvey, Sulas, Dana B., Platt, Heather A. S., Al-Jassim, Mowafak, and Pylypenko, Svitlana. Wed .
"Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in β-Li 3 PS 4 Ceramic Electrolyte". United States. https://doi.org/10.1149/2.0301816jes. https://www.osti.gov/servlets/purl/1492515.
@article{osti_1492515,
title = {Toward All-Solid-State Lithium Batteries: Three-Dimensional Visualization of Lithium Migration in β-Li 3 PS 4 Ceramic Electrolyte},
author = {Seitzman, Natalie and Guthrey, Harvey and Sulas, Dana B. and Platt, Heather A. S. and Al-Jassim, Mowafak and Pylypenko, Svitlana},
abstractNote = {All-solid lithium batteries are an attractive next-generation technology that use ion-conducting solids such as ..beta..-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 um. 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.},
doi = {10.1149/2.0301816jes},
journal = {Journal of the Electrochemical Society},
number = 16,
volume = 165,
place = {United States},
year = {Wed Dec 05 00:00:00 EST 2018},
month = {Wed Dec 05 00:00:00 EST 2018}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 40 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Synchrotron X-ray Analytical Techniques for Studying Materials Electrochemistry in Rechargeable Batteries
journal, September 2017
- Lin, Feng; Liu, Yijin; Yu, Xiqian
- Chemical Reviews, Vol. 117, Issue 21
Electrochemical Deposition and Stripping Behavior of Lithium Metal across a Rigid Block Copolymer Electrolyte Membrane
journal, January 2015
- Harry, Katherine J.; Liao, Xunxun; Parkinson, Dilworth Y.
- Journal of The Electrochemical Society, Vol. 162, Issue 14
On the Detection Limits of Li K X-rays Using Windowless Energy Dispersive Spectrometer (EDS)
journal, July 2017
- Hovington, P.; Timoshevskii, V.; Bessette, S.
- Microscopy and Microanalysis, Vol. 23, Issue S1
Can we detect Li K X-ray in lithium compounds using energy dispersive spectroscopy?: Can we detect Li K X-ray in lithium compounds using EDS?
journal, February 2016
- Hovington, Pierre; Timoshevskii, Vladimir; Burgess, Simon
- Scanning, Vol. 38, Issue 6
Lithium Dendrite Formation on a Lithium Metal Anode from Liquid, Polymer and Solid Electrolytes
journal, January 2016
- Takeda, Yasuo; Yamamoto, Osamu; Imanishi, Nobuyuki
- Electrochemistry, Vol. 84, Issue 4
Synthesis of plate-like Li3PS4 solid electrolyte via liquid-phase shaking for all-solid-state lithium batteries
journal, February 2017
- Phuc, Nguyen Huu Huy; Morikawa, Kei; Mitsuhiro, Totani
- Ionics, Vol. 23, Issue 8
Fabrication of Sub-Micrometer-Thick Solid Electrolyte Membranes of β-Li 3 PS 4 via Tiled Assembly of Nanoscale, Plate-Like Building Blocks
journal, May 2018
- Hood, Zachary D.; Wang, Hui; Pandian, Amaresh Samuthira
- Advanced Energy Materials, Vol. 8, Issue 21
Influence of Electrolyte Modulus on the Local Current Density at a Dendrite Tip on a Lithium Metal Electrode
journal, January 2016
- Harry, Katherine J.; Higa, Kenneth; Srinivasan, Venkat
- Journal of The Electrochemical Society, Vol. 163, Issue 10
Factors Which Limit the Cycle Life of Rechargeable Lithium (Metal) Batteries
journal, January 2000
- Aurbach, D.; Zinigrad, E.; Teller, H.
- Journal of The Electrochemical Society, Vol. 147, Issue 4
Ceramic and polymeric solid electrolytes for lithium-ion batteries
journal, August 2010
- Fergus, Jeffrey W.
- Journal of Power Sources, Vol. 195, Issue 15, p. 4554-4569
Intergranular Li metal propagation through polycrystalline Li6.25Al0.25La3Zr2O12 ceramic electrolyte
journal, January 2017
- Cheng, Eric Jianfeng; Sharafi, Asma; Sakamoto, Jeff
- Electrochimica Acta, Vol. 223
Recent development of sulfide solid electrolytes and interfacial modification for all-solid-state rechargeable lithium batteries
journal, March 2013
- Tatsumisago, Masahiro; Nagao, Motohiro; Hayashi, Akitoshi
- Journal of Asian Ceramic Societies, Vol. 1, Issue 1
X-Ray Tomography of Porous, Transition Metal Oxide Based Lithium Ion Battery Electrodes
journal, March 2013
- Ebner, Martin; Geldmacher, Felix; Marone, Federica
- Advanced Energy Materials, Vol. 3, Issue 7
New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM
journal, November 2017
- Wang, Xuefeng; Zhang, Minghao; Alvarado, Judith
- Nano Letters, Vol. 17, Issue 12
The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces
journal, January 2005
- Monroe, Charles; Newman, John
- Journal of The Electrochemical Society, Vol. 152, Issue 2
Internal Morphologies of Cycled Li-Metal Electrodes Investigated by Nano-Scale Resolution X-ray Computed Tomography
journal, May 2017
- Frisco, Sarah; Liu, Danny X.; Kumar, Arjun
- ACS Applied Materials & Interfaces, Vol. 9, Issue 22
Do imaging techniques add real value to the development of better post-Li-ion batteries?
journal, January 2018
- Conder, Joanna; Marino, Cyril; Novák, Petr
- Journal of Materials Chemistry A, Vol. 6, Issue 8
Multi Length Scale Microstructural Investigations of a Commercially Available Li-Ion Battery Electrode
journal, January 2012
- Shearing, P. R.; Brandon, N. P.; Gelb, J.
- Journal of The Electrochemical Society, Vol. 159, Issue 7
Limb proportions show developmental plasticity in response to embryo movement
journal, February 2017
- Pollard, A. S.; Charlton, B. G.; Hutchinson, J. R.
- Scientific Reports, Vol. 7, Issue 1
Contact between Garnet-Type Solid Electrolyte and Lithium Metal Anode: Influence on Charge Transfer Resistance and Short Circuit Prevention
journal, January 2017
- Basappa, Rajendra Hongahally; Ito, Tomoko; Yamada, Hirotoshi
- Journal of The Electrochemical Society, Vol. 164, Issue 4
In-operando high-speed tomography of lithium-ion batteries during thermal runaway
journal, April 2015
- Finegan, Donal P.; Scheel, Mario; Robinson, James B.
- Nature Communications, Vol. 6, Issue 1
In operando x-ray tomography for next-generation batteries: a systematic approach to monitor reaction product distribution and transport processes
journal, September 2016
- Schröder, D.; Bender, C. L.; Arlt, T.
- Journal of Physics D: Applied Physics, Vol. 49, Issue 40
Lithium metal anodes for rechargeable batteries
journal, January 2014
- Xu, Wu; Wang, Jiulin; Ding, Fei
- Energy Environ. Sci., Vol. 7, Issue 2
Investigation of failure mechanisms in silicon based half cells during the first cycle by micro X-ray tomography and radiography
journal, July 2016
- Sun, Fu; Markötter, Henning; Dong, Kang
- Journal of Power Sources, Vol. 321
In situ SEM study of a lithium deposition and dissolution mechanism in a bulk-type solid-state cell with a Li2S–P2S5 solid electrolyte
journal, January 2013
- Nagao, Motohiro; Hayashi, Akitoshi; Tatsumisago, Masahiro
- Physical Chemistry Chemical Physics, Vol. 15, Issue 42
Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes
journal, July 2017
- Porz, Lukas; Swamy, Tushar; Sheldon, Brian W.
- Advanced Energy Materials, Vol. 7, Issue 20
Direct observation of lithium dendrites inside garnet-type lithium-ion solid electrolyte
journal, August 2015
- Ren, Yaoyu; Shen, Yang; Lin, Yuanhua
- Electrochemistry Communications, Vol. 57
Anomalous High Ionic Conductivity of Nanoporous β-Li3PS4
journal, January 2013
- Liu, Zengcai; Fu, Wujun; Payzant, E. Andrew
- Journal of the American Chemical Society, Vol. 135, Issue 3, p. 975-978
Works referencing / citing this record:
Stack Pressure Considerations for Room‐Temperature All‐Solid‐State Lithium Metal Batteries
journal, November 2019
- Doux, Jean‐Marie; Nguyen, Han; Tan, Darren H. S.
- Advanced Energy Materials, Vol. 10, Issue 1