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Title: Characterizing the Li–Li 7La 3Zr 2O 12 interface stability and kinetics as a function of temperature and current density

The stability and kinetics of the Li–Li 7La 3Zr 2O 12 (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 cm 2; 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.
 [1] ;  [2] ;  [2] ;  [3] ;  [1]
  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:
Grant/Contract Number:
AC05-00OR22725; AR0000399; EE-00006821
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 302; Journal Issue: C; Journal ID: ISSN 0378-7753
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Country of Publication:
United States
36 MATERIALS SCIENCE; solid state electrolyte; Li; current density; charge transfer
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1359451