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High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes

Author

Listed:
  • Yong-Gun Lee

    (Samsung Electronics Co., Ltd)

  • Satoshi Fujiki

    (Samsung R&D Institute Japan)

  • Changhoon Jung

    (Samsung Electronics Co., Ltd)

  • Naoki Suzuki

    (Samsung R&D Institute Japan)

  • Nobuyoshi Yashiro

    (Samsung R&D Institute Japan)

  • Ryo Omoda

    (Samsung R&D Institute Japan)

  • Dong-Su Ko

    (Samsung Electronics Co., Ltd)

  • Tomoyuki Shiratsuchi

    (Samsung R&D Institute Japan)

  • Toshinori Sugimoto

    (Samsung Electronics Co., Ltd)

  • Saebom Ryu

    (Samsung Electronics Co., Ltd)

  • Jun Hwan Ku

    (Samsung Electronics Co., Ltd)

  • Taku Watanabe

    (Samsung R&D Institute Japan)

  • Youngsin Park

    (Samsung Electronics Co., Ltd)

  • Yuichi Aihara

    (Samsung R&D Institute Japan)

  • Dongmin Im

    (Samsung Electronics Co., Ltd)

  • In Taek Han

    (Samsung Electronics Co., Ltd)

Abstract

An all-solid-state battery with a lithium metal anode is a strong candidate for surpassing conventional lithium-ion battery capabilities. However, undesirable Li dendrite growth and low Coulombic efficiency impede their practical application. Here we report that a high-performance all-solid-state lithium metal battery with a sulfide electrolyte is enabled by a Ag–C composite anode with no excess Li. We show that the thin Ag–C layer can effectively regulate Li deposition, which leads to a genuinely long electrochemical cyclability. In our full-cell demonstrations, we employed a high-Ni layered oxide cathode with a high specific capacity (>210 mAh g−1) and high areal capacity (>6.8 mAh cm−2) and an argyrodite-type sulfide electrolyte. A warm isostatic pressing technique was also introduced to improve the contact between the electrode and the electrolyte. A prototype pouch cell (0.6 Ah) thus prepared exhibited a high energy density (>900 Wh l−1), stable Coulombic efficiency over 99.8% and long cycle life (1,000 times).

Suggested Citation

  • Yong-Gun Lee & Satoshi Fujiki & Changhoon Jung & Naoki Suzuki & Nobuyoshi Yashiro & Ryo Omoda & Dong-Su Ko & Tomoyuki Shiratsuchi & Toshinori Sugimoto & Saebom Ryu & Jun Hwan Ku & Taku Watanabe & Youn, 2020. "High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes," Nature Energy, Nature, vol. 5(4), pages 299-308, April.
  • Handle: RePEc:nat:natene:v:5:y:2020:i:4:d:10.1038_s41560-020-0575-z
    DOI: 10.1038/s41560-020-0575-z
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    Cited by:

    1. Chanho Kim & Gyutae Nam & Yoojin Ahn & Xueyu Hu & Meilin Liu, 2024. "Nb1.60Ti0.32W0.08O5−δ as negative electrode active material for durable and fast-charging all-solid-state Li-ion batteries," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Chao Zhu & Till Fuchs & Stefan A. L. Weber & Felix. H. Richter & Gunnar Glasser & Franjo Weber & Hans-Jürgen Butt & Jürgen Janek & Rüdiger Berger, 2023. "Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    3. Haowen Gao & Xin Ai & Hongchun Wang & Wangqin Li & Ping Wei & Yong Cheng & Siwei Gui & Hui Yang & Yong Yang & Ming-Sheng Wang, 2022. "Visualizing the failure of solid electrolyte under GPa-level interface stress induced by lithium eruption," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Ju-Sik Kim & Gabin Yoon & Sewon Kim & Shoichi Sugata & Nobuyoshi Yashiro & Shinya Suzuki & Myung-Jin Lee & Ryounghee Kim & Michael Badding & Zhen Song & JaeMyung Chang & Dongmin Im, 2023. "Surface engineering of inorganic solid-state electrolytes via interlayers strategy for developing long-cycling quasi-all-solid-state lithium batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Dewu Zeng & Jingming Yao & Long Zhang & Ruonan Xu & Shaojie Wang & Xinlin Yan & Chuang Yu & Lin Wang, 2022. "Promoting favorable interfacial properties in lithium-based batteries using chlorine-rich sulfide inorganic solid-state electrolytes," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
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    10. Hyeokjin Kwon & Hyun-Ji Choi & Jung-kyu Jang & Jinhong Lee & Jinkwan Jung & Wonjun Lee & Youngil Roh & Jaewon Baek & Dong Jae Shin & Ju-Hyuk Lee & Nam-Soon Choi & Ying Shirley Meng & Hee-Tak Kim, 2023. "Weakly coordinated Li ion in single-ion-conductor-based composite enabling low electrolyte content Li-metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    11. Yoon, Da Hye & Park, Yong Joon, 2022. "Effects of lithium bis(oxalato)borate-derived surface coating layers on the performances of high-Ni cathodes for all-solid-state batteries," Applied Energy, Elsevier, vol. 326(C).
    12. Burak Aktekin & Luise M. Riegger & Svenja-K. Otto & Till Fuchs & Anja Henss & Jürgen Janek, 2023. "SEI growth on Lithium metal anodes in solid-state batteries quantified with coulometric titration time analysis," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    13. Yuzhao Liu & Xiangyu Meng & Zhiyu Wang & Jieshan Qiu, 2022. "Development of quasi-solid-state anode-free high-energy lithium sulfide-based batteries," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    14. So-Yeon Ham & Elias Sebti & Ashley Cronk & Tyler Pennebaker & Grayson Deysher & Yu-Ting Chen & Jin An Sam Oh & Jeong Beom Lee & Min Sang Song & Phillip Ridley & Darren H. S. Tan & Raphaële J. Clément , 2024. "Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    15. Qian Wu & Mandi Fang & Shizhe Jiao & Siyuan Li & Shichao Zhang & Zeyu Shen & Shulan Mao & Jiale Mao & Jiahui Zhang & Yuanzhong Tan & Kang Shen & Jiaxing Lv & Wei Hu & Yi He & Yingying Lu, 2023. "Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    16. Xiao Zhan & Miao Li & Xiaolin Zhao & Yaning Wang & Sha Li & Weiwei Wang & Jiande Lin & Zi-Ang Nan & Jiawei Yan & Zhefei Sun & Haodong Liu & Fei Wang & Jiayu Wan & Jianjun Liu & Qiaobao Zhang & Li Zhan, 2024. "Self-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    17. Hui Pan & Lei Wang & Yu Shi & Chuanchao Sheng & Sixie Yang & Ping He & Haoshen Zhou, 2024. "A solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    18. Ryan S. Longchamps & Shanhai Ge & Zachary J. Trdinich & Jie Liao & Chao-Yang Wang, 2024. "Battery electronification: intracell actuation and thermal management," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    19. Jing Li & Jizhen Qi & Feng Jin & Fengrui Zhang & Lei Zheng & Lingfei Tang & Rong Huang & Jingjing Xu & Hongwei Chen & Ming Liu & Yejun Qiu & Andrew I. Cooper & Yanbin Shen & Liwei Chen, 2022. "Room temperature all-solid-state lithium batteries based on a soluble organic cage ionic conductor," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    20. Pushun Lu & Yu Xia & Guochen Sun & Dengxu Wu & Siyuan Wu & Wenlin Yan & Xiang Zhu & Jiaze Lu & Quanhai Niu & Shaochen Shi & Zhengju Sha & Liquan Chen & Hong Li & Fan Wu, 2023. "Realizing long-cycling all-solid-state Li-In||TiS2 batteries using Li6+xMxAs1-xS5I (M=Si, Sn) sulfide solid electrolytes," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    21. Ziteng Liang & Yuxuan Xiang & Kangjun Wang & Jianping Zhu & Yanting Jin & Hongchun Wang & Bizhu Zheng & Zirong Chen & Mingming Tao & Xiangsi Liu & Yuqi Wu & Riqiang Fu & Chunsheng Wang & Martin Winter, 2023. "Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    22. Sunyoung Lee & Hayoung Park & Jae Young Kim & Jihoon Kim & Min-Ju Choi & Sangwook Han & Sewon Kim & Wonju Kim & Ho Won Jang & Jungwon Park & Kisuk Kang, 2024. "Unveiling crystal orientation-dependent interface property in composite cathodes for solid-state batteries by in situ microscopic probe," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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