Open Access
Open access
Nature Communications, volume 13, issue 1, publication number 7638

Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries

Sung-Kyun Jung 1, 2
Hyeokjo Gwon 1
Hyungsub Kim 3
Gabin Yoon 1
Dongki Shin 4
Jihyun Hong 4
Changhoon Jung 5
Ju-Sik Kim 1
Publication typeJournal Article
Publication date2022-12-10
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor16.6
ISSN20411723, 20411723
General Chemistry
General Biochemistry, Genetics and Molecular Biology
Multidisciplinary
General Physics and Astronomy
Abstract

Garnet-type Li7La3Zr2O12 (LLZO) solid electrolytes (SE) demonstrates appealing ionic conductivity properties for all-solid-state lithium metal battery applications. However, LLZO (electro)chemical stability in contact with the lithium metal electrode is not satisfactory for developing practical batteries. To circumvent this issue, we report the preparation of various doped cubic-phase LLZO SEs without vacancy formation (i.e., Li = 7.0 such as Li7La3Zr0.5Hf0.5Sc0.5Nb0.5O12 and Li7La3Zr0.4Hf0.4Sn0.4Sc0.4Ta0.4O12). The entropy-driven synthetic approach allows access to hidden chemical space in cubic-phase garnet and enables lower solid-state synthesis temperature as the cubic-phase nucleation decreases from 750 to 400 °C. We demonstrate that the SEs with Li = 7.0 show better reduction stability against lithium metal compared to SE with low lithium contents and identical atomic species (i.e., Li = 6.6 such as Li6.6La3Zr0.4Hf0.4Sn0.4Sc0.2Ta0.6O12). Moreover, when a Li7La3Zr0.4Hf0.4Sn0.4Sc0.4Ta0.4O12 pellet is tested at 60 °C in coin cell configuration with a Li metal negative electrode, a LiNi1/3Co1/3Mn1/3O2-based positive electrode and an ionic liquid-based electrolyte at the cathode|SE interface, discharge capacity retention of about 92% is delivered after 700 cycles at 0.8 mA/cm2 and 60 °C.

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GOST Copy
Jung S. et al. Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries // Nature Communications. 2022. Vol. 13. No. 1. 7638
GOST all authors (up to 50) Copy
Jung S., Gwon H., Kim H., Yoon G., Shin D., Hong J., Jung C., Kim J. Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries // Nature Communications. 2022. Vol. 13. No. 1. 7638
RIS |
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RIS Copy
TY - JOUR
DO - 10.1038/s41467-022-35287-1
UR - https://doi.org/10.1038/s41467-022-35287-1
TI - Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries
T2 - Nature Communications
AU - Jung, Sung-Kyun
AU - Gwon, Hyeokjo
AU - Kim, Hyungsub
AU - Yoon, Gabin
AU - Shin, Dongki
AU - Hong, Jihyun
AU - Jung, Changhoon
AU - Kim, Ju-Sik
PY - 2022
DA - 2022/12/10 00:00:00
PB - Springer Nature
IS - 1
VL - 13
SN - 2041-1723
SN - 2041-1723
ER -
BibTex
Cite this
BibTex Copy
@article{2022_Jung,
author = {Sung-Kyun Jung and Hyeokjo Gwon and Hyungsub Kim and Gabin Yoon and Dongki Shin and Jihyun Hong and Changhoon Jung and Ju-Sik Kim},
title = {Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries},
journal = {Nature Communications},
year = {2022},
volume = {13},
publisher = {Springer Nature},
month = {dec},
url = {https://doi.org/10.1038/s41467-022-35287-1},
number = {1},
doi = {10.1038/s41467-022-35287-1}
}
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