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Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Author

Listed:
  • Weijiang Xue

    (Massachusetts Institute of Technology)

  • Mingjun Huang

    (Massachusetts Institute of Technology)

  • Yutao Li

    (University of Texas at Austin)

  • Yun Guang Zhu

    (Massachusetts Institute of Technology)

  • Rui Gao

    (Massachusetts Institute of Technology)

  • Xianghui Xiao

    (Brookhaven National Laboratory)

  • Wenxu Zhang

    (Massachusetts Institute of Technology)

  • Sipei Li

    (Massachusetts Institute of Technology)

  • Guiyin Xu

    (Massachusetts Institute of Technology)

  • Yang Yu

    (Massachusetts Institute of Technology)

  • Peng Li

    (Massachusetts Institute of Technology)

  • Jeffrey Lopez

    (Massachusetts Institute of Technology)

  • Daiwei Yu

    (Massachusetts Institute of Technology)

  • Yanhao Dong

    (Massachusetts Institute of Technology)

  • Weiwei Fan

    (Massachusetts Institute of Technology)

  • Zhe Shi

    (Massachusetts Institute of Technology)

  • Rui Xiong

    (Massachusetts Institute of Technology
    Beijing Institute of Technology)

  • Cheng-Jun Sun

    (Argonne National Laboratory)

  • Inhui Hwang

    (Argonne National Laboratory)

  • Wah-Keat Lee

    (Brookhaven National Laboratory)

  • Yang Shao-Horn

    (Massachusetts Institute of Technology
    Massachusetts Institute of Technology
    Massachusetts Institute of Technology)

  • Jeremiah A. Johnson

    (Massachusetts Institute of Technology)

  • Ju Li

    (Massachusetts Institute of Technology
    Massachusetts Institute of Technology)

Abstract

By increasing the charging voltage, a cell specific energy of >400 W h kg−1 is achievable with LiNi0.8Mn0.1Co0.1O2 in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g−1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.

Suggested Citation

  • Weijiang Xue & Mingjun Huang & Yutao Li & Yun Guang Zhu & Rui Gao & Xianghui Xiao & Wenxu Zhang & Sipei Li & Guiyin Xu & Yang Yu & Peng Li & Jeffrey Lopez & Daiwei Yu & Yanhao Dong & Weiwei Fan & Zhe , 2021. "Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte," Nature Energy, Nature, vol. 6(5), pages 495-505, May.
    • Handle: RePEc:nat:natene:v:6:y:2021:i:5:d:10.1038_s41560-021-00792-y
    DOI: 10.1038/s41560-021-00792-y
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    Cited by:

    1. Zheng Li & Harsha Rao & Rasha Atwi & Bhuvaneswari M. Sivakumar & Bharat Gwalani & Scott Gray & Kee Sung Han & Thomas A. Everett & Tanvi A. Ajantiwalay & Vijayakumar Murugesan & Nav Nidhi Rajput & Vila, 2023. "Non-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    2. Yao Wang & Shuyu Dong & Yifu Gao & Pui-Kit Lee & Yao Tian & Yuefeng Meng & Xia Hu & Xin Zhao & Baohua Li & Dong Zhou & Feiyu Kang, 2024. "Difluoroester solvent toward fast-rate anion-intercalation lithium metal batteries under extreme conditions," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. Junbo Zhang & Haikuo Zhang & Suting Weng & Ruhong Li & Di Lu & Tao Deng & Shuoqing Zhang & Ling Lv & Jiacheng Qi & Xuezhang Xiao & Liwu Fan & Shujiang Geng & Fuhui Wang & Lixin Chen & Malachi Noked & , 2023. "Multifunctional solvent molecule design enables high-voltage Li-ion batteries," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    4. Kai Wang & Zhenqi Gu & Zhiwei Xi & Lv Hu & Cheng Ma, 2023. "Li3TiCl6 as ionic conductive and compressible positive electrode active material for all-solid-state lithium-based batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Danfeng Zhang & Ming Liu & Jiabin Ma & Ke Yang & Zhen Chen & Kaikai Li & Chen Zhang & Yinping Wei & Min Zhou & Peng Wang & Yuanbiao He & Wei Lv & Quan-Hong Yang & Feiyu Kang & Yan-Bing He, 2022. "Lithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    6. Guangzhao Zhang & Jian Chang & Liguang Wang & Jiawei Li & Chaoyang Wang & Ruo Wang & Guoli Shi & Kai Yu & Wei Huang & Honghe Zheng & Tianpin Wu & Yonghong Deng & Jun Lu, 2023. "A monofluoride ether-based electrolyte solution for fast-charging and low-temperature non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Minglei Mao & Xiao Ji & Qiyu Wang & Zejing Lin & Meiying Li & Tao Liu & Chengliang Wang & Yong-Sheng Hu & Hong Li & Xuejie Huang & Liquan Chen & Liumin Suo, 2023. "Anion-enrichment interface enables high-voltage anode-free lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
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    9. Shuoqing Zhang & Ruhong Li & Nan Hu & Tao Deng & Suting Weng & Zunchun Wu & Di Lu & Haikuo Zhang & Junbo Zhang & Xuefeng Wang & Lixin Chen & Liwu Fan & Xiulin Fan, 2022. "Tackling realistic Li+ flux for high-energy lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    10. Matthew Sadd & Shizhao Xiong & Jacob R. Bowen & Federica Marone & Aleksandar Matic, 2023. "Investigating microstructure evolution of lithium metal during plating and stripping via operando X-ray tomographic microscopy," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    11. Wenda Li & Hengyue Xu & Hongyi Zhang & Facai Wei & Lingyan Huang & Shanzhe Ke & Jianwei Fu & Chengbin Jing & Jiangong Cheng & Shaohua Liu, 2023. "Tuning electron delocalization of hydrogen-bonded organic framework cathode for high-performance zinc-organic batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    12. Zhuo Li & Rui Yu & Suting Weng & Qinghua Zhang & Xuefeng Wang & Xin Guo, 2023. "Tailoring polymer electrolyte ionic conductivity for production of low- temperature operating quasi-all-solid-state lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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