Inorganic Chemistry, volume 50, issue 3, pages 1089-1097

Crystal Chemistry and Stability of “Li₇La₃Zr₂O₁₂” Garnet: A Fast Lithium-Ion Conductor

Charles A. Geiger ¹

E. Alekseev ¹

Biljana Lazic ²

Martin Fisch ²

Thomas Armbrüster ²

Ramona Langner ³

Michael Fechtelkord ³

Namjun Kim ⁴

T. Pettke ²

Werner Weppner ⁵

Hide authors affiliations Show authors affiliations: 5 affiliations

Institut für Geowissenschaften, Abteilung Mineralogie, Christian-Albrechts-Universität zu Kiel, D-24118 Kiel, Germany |

Mineralogische Kristallographie, Institut für Geologie, Universität Bern, CH-3012 Bern, Switzerland |

Institut für Geologie, Mineralogie und Geophysik, Ruhr-Universität Bochum, D-44780 Bochum, Germany |

⁴

Department of Geological and Environmental Sciences, Stanford University, Stanford, California 94305-2115, United States |

⁵

Institut für Anorganische Chemie, Christian-Albrechts-Universität zu Kiel, Otto-Hahn-Platz 6-7, D-24118 Kiel, Germany |

Publication type: Journal Article

Publication date: 2010-12-28

American Chemical Society (ACS)

Journal: Inorganic Chemistry

Quartile SCImago

Quartile WOS

Impact factor: 4.6

ISSN: 00201669, 1520510X

DOI: 10.1021/ic101914e

Copy DOI

Inorganic Chemistry

Physical and Theoretical Chemistry

Abstract

Recent research has shown that certain Li-oxide garnets with high mechanical, thermal, chemical, and electrochemical stability are excellent fast Li-ion conductors. However, the detailed crystal chemistry of Li-oxide garnets is not well understood, nor is the relationship between crystal chemistry and conduction behavior. An investigation was undertaken to understand the crystal chemical and structural properties, as well as the stability relations, of Li7La3Zr2O12 garnet, which is the best conducting Li-oxide garnet discovered to date. Two different sintering methods produced Li-oxide garnet but with slightly different compositions and different grain sizes. The first sintering method, involving ceramic crucibles in initial synthesis steps and later sealed Pt capsules, produced single crystals up to roughly 100 μm in size. Electron microprobe and laser ablation inductively coupled plasma mass spectrometry (ICP-MS) measurements show small amounts of Al in the garnet, probably originating from the crucibles. The crystal structure of this phase was determined using X-ray single-crystal diffraction every 100 K from 100 K up to 500 K. The crystals are cubic with space group Ia3̅d at all temperatures. The atomic displacement parameters and Li-site occupancies were measured. Li atoms could be located on at least two structural sites that are partially occupied, while other Li atoms in the structure appear to be delocalized. 27Al NMR spectra show two main resonances that are interpreted as indicating that minor Al occurs on the two different Li sites. Li NMR spectra show a single narrow resonance at 1.2−1.3 ppm indicating fast Li-ion diffusion at room temperature. The chemical shift value indicates that the Li atoms spend most of their time at the tetrahedrally coordinated C (24d) site. The second synthesis method, using solely Pt crucibles during sintering, produced fine-grained Li7La3Zr2O12 crystals. This material was studied by X-ray powder diffraction at different temperatures between 25 and 200 °C. This phase is tetragonal at room temperature and undergoes a phase transition to a cubic phase between 100 and 150 °C. Cubic “Li7La3Zr2O12” may be stabilized at ambient conditions relative to its slightly less conducting tetragonal modification via small amounts of Al3+. Several crystal chemical properties appear to promote the high Li-ion conductivity in cubic Al-containing Li7La3Zr2O12. They are (i) isotropic three-dimensional Li-diffusion pathways, (ii) closely spaced Li sites and Li delocalization that allow for easy and fast Li diffusion, and (iii) low occupancies at the Li sites, which may also be enhanced by the heterovalent substitution Al3+ ⇔ 3Li.

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Geiger C. A. et al. Crystal Chemistry and Stability of “Li7La3Zr2O12” Garnet: A Fast Lithium-Ion Conductor // Inorganic Chemistry. 2010. Vol. 50. No. 3. pp. 1089-1097.

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Geiger C. A., Alekseev E., Lazic B., Fisch M., Armbrüster T., Langner R., Fechtelkord M., Kim N., Pettke T., Weppner W. Crystal Chemistry and Stability of “Li7La3Zr2O12” Garnet: A Fast Lithium-Ion Conductor // Inorganic Chemistry. 2010. Vol. 50. No. 3. pp. 1089-1097.

RIS |

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RIS Copy

TY - JOUR

DO - 10.1021/ic101914e

UR - https://doi.org/10.1021/ic101914e

TI - Crystal Chemistry and Stability of “Li7La3Zr2O12” Garnet: A Fast Lithium-Ion Conductor

T2 - Inorganic Chemistry

AU - Lazic, Biljana

AU - Fisch, Martin

AU - Armbrüster, Thomas

AU - Langner, Ramona

AU - Kim, Namjun

AU - Weppner, Werner

AU - Geiger, Charles A.

AU - Alekseev, E.

AU - Fechtelkord, Michael

AU - Pettke, T.

PY - 2010

DA - 2010/12/28 00:00:00

PB - American Chemical Society (ACS)

SP - 1089-1097

IS - 3

VL - 50

SN - 0020-1669

SN - 1520-510X

ER -

BibTex |

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@article{2010_Geiger,

author = {Biljana Lazic and Martin Fisch and Thomas Armbrüster and Ramona Langner and Namjun Kim and Werner Weppner and Charles A. Geiger and E. Alekseev and Michael Fechtelkord and T. Pettke},

title = {Crystal Chemistry and Stability of “Li7La3Zr2O12” Garnet: A Fast Lithium-Ion Conductor},

journal = {Inorganic Chemistry},

year = {2010},

volume = {50},

publisher = {American Chemical Society (ACS)},

month = {dec},

url = {https://doi.org/10.1021/ic101914e},

number = {3},

pages = {1089--1097},

doi = {10.1021/ic101914e}

}

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MLA Copy

Geiger, Charles A., et al. “Crystal Chemistry and Stability of “Li7La3Zr2O12” Garnet: A Fast Lithium-Ion Conductor.” Inorganic Chemistry, vol. 50, no. 3, Dec. 2010, pp. 1089-1097. https://doi.org/10.1021/ic101914e.

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Publisher

American Chemical Society (ACS)

Journal

Inorganic Chemistry

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Quartile WOS

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4.6

ISSN

00201669 (Print)
1520510X (Electronic)