Clarifying the Dopant Local Structure and Effect on Ionic Conductivity in Garnet Solid-State Electrolytes for Lithium-Ion Batteries Article Swipe
Sundeep Vema
,
Astrid H. Berge
,
Supreeth Nagendran
,
Clare P. Grey
·
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/acs.chemmater.3c01831
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/acs.chemmater.3c01831
The high Li-ion conductivity and wide electrochemical stability of Li-rich garnets (Li7La3Zr2O12) make them one of the leading solid electrolyte candidates for solid-state batteries. Dopants such as Al and Ga are typically used to enable stabilisation of the high Li+ ion-conductive cubic phase at room temperature. Although numerous studies exist that have characterized the electrochemical properties, structure, and lithium diffusion in Al- and GaLLZO, the local structure and site occupancy of dopants in these compounds are not well understood. Two broad 27Al or 69,71Ga resonances are often observed with chemical shifts consistent with tetrahedrally coordinated Al/Ga in the magic angle spinning nuclear magnetic resonance (MAS-NMR) spectra of both Al- and Ga-LLZO, which have been assigned to either Al and/or Ga occupying 24d and 96h/48g sites in the LLZO lattice or to the different Al/Ga configurations that arise from different arrangements of Li around these dopants. In this work, we unambiguously show that the side products γ-LiAlO2 and LiGaO2 lead to the high frequency resonances observed by NMR spectroscopy and that both Al and Ga only occupy the 24d site in the LLZO lattice. Furthermore, it was observed that the excess Li often used during synthesis leads to the formation of these side-products by consuming the Al/Ga dopants. In addition, the consumption of Al/Ga dopants lead to the tetragonal phase formation commonly observed in the literature, even after careful mixing of precursors. The side-products can exist even after sintering, thus controlling the Al/Ga content in the LLZO lattice substantially influences the lithium-ion conductivity in LLZO, as measured here by electrochemical impedance spectroscopy.
Related Topics
Concepts
Dopant
Tetragonal crystal system
Materials science
Ionic conductivity
Lithium (medication)
Fast ion conductor
Magic angle spinning
Conductivity
Ion
Ionic bonding
Solid-state nuclear magnetic resonance
Electrolyte
Doping
Chemical physics
Crystal structure
Crystallography
Chemistry
Nuclear magnetic resonance spectroscopy
Nuclear magnetic resonance
Physical chemistry
Stereochemistry
Organic chemistry
Physics
Optoelectronics
Endocrinology
Electrode
Medicine
Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acs.chemmater.3c01831
- OA Status
- hybrid
- Cited By
- 26
- References
- 64
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4388654300
All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
-
https://openalex.org/W4388654300Canonical identifier for this work in OpenAlex
- DOI
-
https://doi.org/10.1021/acs.chemmater.3c01831Digital Object Identifier
- Title
-
Clarifying the Dopant Local Structure and Effect on Ionic Conductivity in Garnet Solid-State Electrolytes for Lithium-Ion BatteriesWork title
- Type
-
articleOpenAlex work type
- Language
-
enPrimary language
- Publication year
-
2023Year of publication
- Publication date
-
2023-11-14Full publication date if available
- Authors
-
Sundeep Vema, Astrid H. Berge, Supreeth Nagendran, Clare P. GreyList of authors in order
- Landing page
-
https://doi.org/10.1021/acs.chemmater.3c01831Publisher landing page
- Open access
-
YesWhether a free full text is available
- OA status
-
hybridOpen access status per OpenAlex
- OA URL
-
https://doi.org/10.1021/acs.chemmater.3c01831Direct OA link when available
- Concepts
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Dopant, Tetragonal crystal system, Materials science, Ionic conductivity, Lithium (medication), Fast ion conductor, Magic angle spinning, Conductivity, Ion, Ionic bonding, Solid-state nuclear magnetic resonance, Electrolyte, Doping, Chemical physics, Crystal structure, Crystallography, Chemistry, Nuclear magnetic resonance spectroscopy, Nuclear magnetic resonance, Physical chemistry, Stereochemistry, Organic chemistry, Physics, Optoelectronics, Endocrinology, Electrode, MedicineTop concepts (fields/topics) attached by OpenAlex
- Cited by
-
26Total citation count in OpenAlex
- Citations by year (recent)
-
2025: 15, 2024: 10, 2023: 1Per-year citation counts (last 5 years)
- References (count)
-
64Number of works referenced by this work
- Related works (count)
-
10Other works algorithmically related by OpenAlex
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