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

Sung-Kyun Jung (), Hyeokjo Gwon (), Hyungsub Kim, Gabin Yoon, Dongki Shin, Jihyun Hong, Changhoon Jung and Ju-Sik Kim
Additional contact information
Sung-Kyun Jung: Samsung Electronics Co., Ltd.
Hyeokjo Gwon: Samsung Electronics Co., Ltd.
Hyungsub Kim: Korea Atomic Energy Research Institute (KAERI)
Gabin Yoon: Samsung Electronics Co., Ltd.
Dongki Shin: Korea Institute of Science and Technology (KIST)
Jihyun Hong: Korea Institute of Science and Technology (KIST)
Changhoon Jung: Samsung Electronics Co., Ltd.
Ju-Sik Kim: Samsung Electronics Co., Ltd.

Nature Communications, 2022, vol. 13, issue 1, 1-13

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-35287-1

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