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Effects of Al concentration on the structure and conductivity of lithium lanthanum zirconium oxide

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/d4ta04862h· OSTI ID:2474732
 [1];  [2];  [3];  [4];  [2];  [5]
  1. Univ. of Michigan, Ann Arbor, MI (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States)
  5. Univ. of Michigan, Ann Arbor, MI (United States); Univ. of California, Santa Barbara, CA (United States)
Cubic Li7-3xAlxLa3Zr2O12 (LLZO) is a promising, next-generation solid electrolyte due to its stability with Li-metal and high bulk conductivity (~1 mS cm-1). However, the source of the high conductivity is not completely understood. In this work, we address this key knowledge gap through the integration of elemental analysis, neutron diffraction sensitive to Li and O atoms, and impedance spectroscopy to understand the structure–property correlations for LLZO. We show the metal–oxygen framework structure remains constant with variation in Al substitution, resulting in a constant activation energy of ~0.35 eV and little effect on the bulk conductivity. Instead, Li concentration, Al blocking and trapping of mobile defects, and Li–Li nearest neighbor interactions largely control the Al substituted LLZO bulk conductivity, resulting in decreases from 0.73 to 0.22 mS cm-1 as the Al concentration increases from 0.17 to 0.32 mol. These results differ from those of Ta substituted LLZO, where the framework structure and Li–Li site distances play large roles in controlling the conductivity. The increased understanding of the controlling factors of conductivity allows for greater ability to tailor the design of and substitution into the LLZO structure for improved conductivity.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)
Grant/Contract Number:
AC05-00OR22725; SC0014664
OSTI ID:
2474732
Alternate ID(s):
OSTI ID: 2472980
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 41 Vol. 12; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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