Effects of Al concentration on the structure and conductivity of lithium lanthanum zirconium oxide
Journal Article
·
· Journal of Materials Chemistry. A
- Univ. of Michigan, Ann Arbor, MI (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- 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
Similar Records
The effects of aluminum concentration on the microstructural and electrochemical properties of lithium lanthanum zirconium oxide
Irreversible Multielement Diffusion and the Resulting Compositional and Processing Flexibility in the Synthesis and Densification of Lithium Aluminum Lanthanum Zirconium Oxide
Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes
Journal Article
·
Tue Sep 27 20:00:00 EDT 2022
· Journal of Materials Chemistry. A
·
OSTI ID:2423973
Irreversible Multielement Diffusion and the Resulting Compositional and Processing Flexibility in the Synthesis and Densification of Lithium Aluminum Lanthanum Zirconium Oxide
Journal Article
·
Fri Feb 14 19:00:00 EST 2025
· ACS Applied Energy Materials
·
OSTI ID:2538249
Synthesis and characterization of substituted garnet and perovskite-based lithium-ion conducting solid electrolytes
Journal Article
·
Tue Sep 29 20:00:00 EDT 2015
· Ionics
·
OSTI ID:1241462