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Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Author

Listed:
  • Zhiao Yu

    (Stanford University
    Stanford University)

  • Paul E. Rudnicki

    (Stanford University)

  • Zewen Zhang

    (Stanford University)

  • Zhuojun Huang

    (Stanford University)

  • Hasan Celik

    (University of California)

  • Solomon T. Oyakhire

    (Stanford University)

  • Yuelang Chen

    (Stanford University
    Stanford University)

  • Xian Kong

    (Stanford University)

  • Sang Cheol Kim

    (Stanford University)

  • Xin Xiao

    (Stanford University)

  • Hansen Wang

    (Stanford University)

  • Yu Zheng

    (Stanford University
    Stanford University)

  • Gaurav A. Kamat

    (Stanford University)

  • Mun Sek Kim

    (Stanford University
    Stanford University)

  • Stacey F. Bent

    (Stanford University)

  • Jian Qin

    (Stanford University)

  • Yi Cui

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Zhenan Bao

    (Stanford University)

Abstract

Electrolyte engineering improved cycling of Li metal batteries and anode-free cells at low current densities; however, high-rate capability and tuning of ionic conduction in electrolytes are desirable yet less-studied. Here, we design and synthesize a family of fluorinated-1,2-diethoxyethanes as electrolyte solvents. The position and amount of F atoms functionalized on 1,2-diethoxyethane were found to greatly affect electrolyte performance. Partially fluorinated, locally polar –CHF2 is identified as the optimal group rather than fully fluorinated –CF3 in common designs. Paired with 1.2 M lithium bis(fluorosulfonyl)imide, these developed single-salt-single-solvent electrolytes simultaneously enable high conductivity, low and stable overpotential, >99.5% Li||Cu half-cell efficiency (up to 99.9%, ±0.1% fluctuation) and fast activation (Li efficiency >99.3% within two cycles). Combined with high-voltage stability, these electrolytes achieve roughly 270 cycles in 50-μm-thin Li||high-loading-NMC811 full batteries and >140 cycles in fast-cycling Cu||microparticle-LiFePO4 industrial pouch cells under realistic testing conditions. The correlation of Li+–solvent coordination, solvation environments and battery performance is investigated to understand structure–property relationships.

Suggested Citation

  • Zhiao Yu & Paul E. Rudnicki & Zewen Zhang & Zhuojun Huang & Hasan Celik & Solomon T. Oyakhire & Yuelang Chen & Xian Kong & Sang Cheol Kim & Xin Xiao & Hansen Wang & Yu Zheng & Gaurav A. Kamat & Mun Se, 2022. "Rational solvent molecule tuning for high-performance lithium metal battery electrolytes," Nature Energy, Nature, vol. 7(1), pages 94-106, January.
  • Handle: RePEc:nat:natene:v:7:y:2022:i:1:d:10.1038_s41560-021-00962-y
    DOI: 10.1038/s41560-021-00962-y
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    Citations

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    Cited by:

    1. 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.
    2. Zhixin Xu & Xiyue Zhang & Jun Yang & Xuzixu Cui & Yanna Nuli & Jiulin Wang, 2024. "High-voltage and intrinsically safe electrolytes for Li metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. 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.
    4. Jijiang Liu & Wei Hao & Mingming Fang & Xin Chen & Yongteng Dong & Yuanmao Chen & Zhiyong Wang & Xinyang Yue & Zheng Liang, 2024. "Screening of F-containing electrolyte additives and clarifying their decomposition routes for stable Li metal anodes," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Muhammad Mominur Rahman & Sha Tan & Yang Yang & Hui Zhong & Sanjit Ghose & Iradwikanari Waluyo & Adrian Hunt & Lu Ma & Xiao-Qing Yang & Enyuan Hu, 2023. "An inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Yangyang Feng & Yong Li & Jing Lin & Huyue Wu & Lei Zhu & Xiang Zhang & Linlin Zhang & Chuan-Fu Sun & Maoxiang Wu & Yaobing Wang, 2023. "Production of high-energy 6-Ah-level Li | |LiNi0.83Co0.11Mn0.06O2 multi-layer pouch cells via negative electrode protective layer coating strategy," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    7. Jiawei Chen & Daoming Zhang & Lei Zhu & Mingzhu Liu & Tianle Zheng & Jie Xu & Jun Li & Fei Wang & Yonggang Wang & Xiaoli Dong & Yongyao Xia, 2024. "Hybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    8. 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.
    9. Yanfei Zhu & Zhoujie Lao & Mengtian Zhang & Tingzheng Hou & Xiao Xiao & Zhihong Piao & Gongxun Lu & Zhiyuan Han & Runhua Gao & Lu Nie & Xinru Wu & Yanze Song & Chaoyuan Ji & Jian Wang & Guangmin Zhou, 2024. "A locally solvent-tethered polymer electrolyte for long-life lithium metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    10. Fangli Zhang & Wenchao Zhang & Jodie A. Yuwono & David Wexler & Yameng Fan & Jinshuo Zou & Gemeng Liang & Liang Sun & Zaiping Guo, 2024. "Catalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    11. Hyeokjin Kwon & Hongsin Kim & Jaemin Hwang & Wonsik Oh & Youngil Roh & Dongseok Shin & Hee-Tak Kim, 2024. "Borate–pyran lean electrolyte-based Li-metal batteries with minimal Li corrosion," Nature Energy, Nature, vol. 9(1), pages 57-69, January.
    12. 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.
    13. Yanhua Zhang & Rui Qiao & Qiaona Nie & Peiyu Zhao & Yong Li & Yunfei Hong & Shengjie Chen & Chao Li & Baoyu Sun & Hao Fan & Junkai Deng & Jingying Xie & Feng Liu & Jiangxuan Song, 2024. "Synergetic regulation of SEI mechanics and crystallographic orientation for stable lithium metal pouch cells," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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