Jung, Sung-Kyun Gwon, Hyeokjo Kim, Hyungsub Yoon, Gabin Shin, Dongki Hong, Jihyun Jung, Changhoon Kim, Ju-Sik 2024-01-12T02:34:02Z 2024-01-12T02:34:02Z 2023-01-04 2022-12 2041-1723 https://pubs.kist.re.kr/handle/201004/75879 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. English Nature Publishing Group Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries Article 10.1038/s41467-022-35287-1 1 Nature Communications, v.13, no.1 Nature Communications 13 1 Y scie scopus 000971718200008 Multidisciplinary Sciences Science & Technology - Other Topics Article LI-ION CONDUCTION CRYSTAL-STRUCTURE LI7LA3ZR2O12 STABILITY 1ST-PRINCIPLES MECHANISMS INTERFACE LLZO