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Title: 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:
 [1];  [2];  [2];  [3];  [2];  [1]
  1. Colorado School of Mines, Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. 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:
Journal Article: 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. doi: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. doi:10.1149/2.0301816jes.
@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},
issn = {0013-4651},
number = 16,
volume = 165,
place = {United States},
year = {2018},
month = {12}
}

Journal Article:
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Works referenced in this record:

Ceramic and polymeric solid electrolytes for lithium-ion batteries
journal, August 2010


Anomalous High Ionic Conductivity of Nanoporous ?-Li3PS4
journal, January 2013

  • Liu, Zengcai; Fu, Wujun; Payzant, E. Andrew
  • Journal of the American Chemical Society, Vol. 135, Issue 3, p. 975-978
  • DOI: 10.1021/ja3110895