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

Journal Article · · Journal of Power Sources
 [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)
+ Show Author Affiliations

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AC05-00OR22725; AR0000399; EE-00006821
OSTI ID:
1327687
Alternate ID(s):
OSTI ID: 1359451
Journal Information:
Journal of Power Sources, Vol. 302, Issue C; ISSN 0378-7753
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 357 works
Citation information provided by
Web of Science

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Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries journal February 2018
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Dendrite nucleation in lithium-conductive ceramics journal January 2019
Sur-/interfacial regulation in all-solid-state rechargeable Li-ion batteries based on inorganic solid-state electrolytes: advances and perspectives journal January 2019
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Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface journal April 2017
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Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer journal April 2017
Free-standing transition metal oxide electrode architectures for electrochemical energy storage journal July 2019
Sodium Plating from Na‐β″‐Alumina Ceramics at Room Temperature, Paving the Way for Fast‐Charging All‐Solid‐State Batteries journal December 2019
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Electrochemical Stability of Li6.5La3Zr1.5M0.5O12 (M = Nb or Ta) against Metallic Lithium journal May 2016

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36 MATERIALS SCIENCE
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