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

Author

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  • Sung-Kyun Jung

    (Samsung Electronics Co., Ltd.
    Ulsan National Institute of Science and Technology (UNIST))

  • 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.)

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.

Suggested Citation

  • Sung-Kyun Jung & Hyeokjo Gwon & Hyungsub Kim & Gabin Yoon & Dongki Shin & Jihyun Hong & Changhoon Jung & Ju-Sik Kim, 2022. "Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35287-1
    DOI: 10.1038/s41467-022-35287-1
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    1. Sewon Kim & Ju-Sik Kim & Lincoln Miara & Yan Wang & Sung-Kyun Jung & Seong Yong Park & Zhen Song & Hyungsub Kim & Michael Badding & JaeMyung Chang & Victor Roev & Gabin Yoon & Ryounghee Kim & Jung-Hwa, 2022. "High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Moran Balaish & Juan Carlos Gonzalez-Rosillo & Kun Joong Kim & Yuntong Zhu & Zachary D. Hood & Jennifer L. M. Rupp, 2021. "Processing thin but robust electrolytes for solid-state batteries," Nature Energy, Nature, vol. 6(3), pages 227-239, March.
    3. Christina M. Rost & Edward Sachet & Trent Borman & Ali Moballegh & Elizabeth C. Dickey & Dong Hou & Jacob L. Jones & Stefano Curtarolo & Jon-Paul Maria, 2015. "Entropy-stabilized oxides," Nature Communications, Nature, vol. 6(1), pages 1-8, December.
    4. Simon Randau & Dominik A. Weber & Olaf Kötz & Raimund Koerver & Philipp Braun & André Weber & Ellen Ivers-Tiffée & Torben Adermann & Jörn Kulisch & Wolfgang G. Zeier & Felix H. Richter & Jürgen Janek, 2020. "Benchmarking the performance of all-solid-state lithium batteries," Nature Energy, Nature, vol. 5(3), pages 259-270, March.
    5. Fei Zhang & Yuan Wu & Hongbo Lou & Zhidan Zeng & Vitali B. Prakapenka & Eran Greenberg & Yang Ren & Jinyuan Yan & John S. Okasinski & Xiongjun Liu & Yong Liu & Qiaoshi Zeng & Zhaoping Lu, 2017. "Polymorphism in a high-entropy alloy," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
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    1. Can Yildirim & Florian Flatscher & Steffen Ganschow & Alice Lassnig & Christoph Gammer & Juraj Todt & Jozef Keckes & Daniel Rettenwander, 2024. "Understanding the origin of lithium dendrite branching in Li6.5La3Zr1.5Ta0.5O12 solid-state electrolyte via microscopy measurements," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    2. Bin Ouyang & Yan Zeng, 2024. "The rise of high-entropy battery materials," Nature Communications, Nature, vol. 15(1), pages 1-5, December.
    3. Zhenyou Song & Tengrui Wang & Hua Yang & Wang Hay Kan & Yuwei Chen & Qian Yu & Likuo Wang & Yini Zhang & Yiming Dai & Huaican Chen & Wen Yin & Takashi Honda & Maxim Avdeev & Henghui Xu & Jiwei Ma & Yu, 2024. "Promoting high-voltage stability through local lattice distortion of halide solid electrolytes," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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