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Title: Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density

Abstract

The stability and kinetics of the Li–Li7La3Zr2O12 (LLZO) interface were characterized as a function of temperature and current density. Polycrystalline LLZO was densified using a rapid hot-pressing technique achieving 97 ± 1% relative density, and <10% grain boundary resistance; effectively consisting of an ensemble of single LLZO crystals. It was determined that by heating to 175 °C, the room temperature Li-LLZO interface resistance decreases dramatically from 5822 (as-assembled) to 514 Ω cm2; a > 10-fold decrease. In characterizing the maximum sustainable current density (or critical current density – CCD) of the Li-LLZO interface, several signs of degradation were observed. In DC cycling tests, significant deviation from Ohmic behavior was observed. In post-cycling tests, regions of metallic Li were observed; propagating parallel to the ionic current. For the cells cycled at 30, 70, 100, 130 and 160 °C, the CCD was determined to be 50, 200, 800, 3500, and 20000 μA cm–2, respectively. As a result, the relationships and phenomena observed in this work can be used to better understand the Li-LLZO interface stability, enabling the use of batteries employing Li metal anodes.

Authors:
 [1];  [2];  [2];  [3];  [1]
+ Show Author Affiliations
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. RDRL-SED-C Army Research Lab., Adelphi, MD (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1327687
Alternate Identifier(s):
OSTI ID: 1359451
Grant/Contract Number:  
AC05-00OR22725; AR0000399; EE-00006821
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 302; Journal Issue: C; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; solid state electrolyte; Li; current density; charge transfer

Citation Formats

Sharafi, Asma, Meyer, Harry M., Nanda, Jagjit, Wolfenstine, Jeff, and Sakamoto, Jeff. Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density. United States: N. p., 2015. Web. doi:10.1016/j.jpowsour.2015.10.053.
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Sharafi, Asma, Meyer, Harry M., Nanda, Jagjit, Wolfenstine, Jeff, & Sakamoto, Jeff. Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density. United States. https://doi.org/10.1016/j.jpowsour.2015.10.053
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Sharafi, Asma, Meyer, Harry M., Nanda, Jagjit, Wolfenstine, Jeff, and Sakamoto, Jeff. Tue . "Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density". United States. https://doi.org/10.1016/j.jpowsour.2015.10.053. https://www.osti.gov/servlets/purl/1327687.
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@article{osti_1327687,
title = {Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density},
author = {Sharafi, Asma and Meyer, Harry M. and Nanda, Jagjit and Wolfenstine, Jeff and Sakamoto, Jeff},
abstractNote = {The stability and kinetics of the Li–Li7La3Zr2O12 (LLZO) interface were characterized as a function of temperature and current density. Polycrystalline LLZO was densified using a rapid hot-pressing technique achieving 97 ± 1% relative density, and <10% grain boundary resistance; effectively consisting of an ensemble of single LLZO crystals. It was determined that by heating to 175 °C, the room temperature Li-LLZO interface resistance decreases dramatically from 5822 (as-assembled) to 514 Ω cm2; a > 10-fold decrease. In characterizing the maximum sustainable current density (or critical current density – CCD) of the Li-LLZO interface, several signs of degradation were observed. In DC cycling tests, significant deviation from Ohmic behavior was observed. In post-cycling tests, regions of metallic Li were observed; propagating parallel to the ionic current. For the cells cycled at 30, 70, 100, 130 and 160 °C, the CCD was determined to be 50, 200, 800, 3500, and 20000 μA cm–2, respectively. As a result, the relationships and phenomena observed in this work can be used to better understand the Li-LLZO interface stability, enabling the use of batteries employing Li metal anodes.},
doi = {10.1016/j.jpowsour.2015.10.053},
journal = {Journal of Power Sources},
number = C,
volume = 302,
place = {United States},
year = {Tue Oct 27 00:00:00 EDT 2015},
month = {Tue Oct 27 00:00:00 EDT 2015}
}
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