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Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries

Author

Listed:
  • Zhiao Yu

    (Stanford University
    Stanford University)

  • Hansen Wang

    (Stanford University)

  • Xian Kong

    (Stanford University)

  • William Huang

    (Stanford University)

  • Yuchi Tsao

    (Stanford University
    Stanford University
    Stanford University)

  • David G. Mackanic

    (Stanford University)

  • Kecheng Wang

    (Stanford University)

  • Xinchang Wang

    (Xiamen University)

  • Wenxiao Huang

    (Stanford University)

  • Snehashis Choudhury

    (Stanford University)

  • Yu Zheng

    (Stanford University
    Stanford University)

  • Chibueze V. Amanchukwu

    (Stanford University)

  • Samantha T. Hung

    (Stanford University)

  • Yuting Ma

    (Stanford University)

  • Eder G. Lomeli

    (Stanford University)

  • Jian Qin

    (Stanford University)

  • Yi Cui

    (Stanford University
    Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory)

  • Zhenan Bao

    (Stanford University)

Abstract

Electrolyte engineering is critical for developing Li metal batteries. While recent works improved Li metal cyclability, a methodology for rational electrolyte design remains lacking. Herein, we propose a design strategy for electrolytes that enable anode-free Li metal batteries with single-solvent single-salt formations at standard concentrations. Rational incorporation of –CF2– units yields fluorinated 1,4-dimethoxylbutane as the electrolyte solvent. Paired with 1 M lithium bis(fluorosulfonyl)imide, this electrolyte possesses unique Li–F binding and high anion/solvent ratio in the solvation sheath, leading to excellent compatibility with both Li metal anodes (Coulombic efficiency ~ 99.52% and fast activation within five cycles) and high-voltage cathodes (~6 V stability). Fifty-μm-thick Li|NMC batteries retain 90% capacity after 420 cycles with an average Coulombic efficiency of 99.98%. Industrial anode-free pouch cells achieve ~325 Wh kg−1 single-cell energy density and 80% capacity retention after 100 cycles. Our design concept for electrolytes provides a promising path to high-energy, long-cycling Li metal batteries.

Suggested Citation

  • Zhiao Yu & Hansen Wang & Xian Kong & William Huang & Yuchi Tsao & David G. Mackanic & Kecheng Wang & Xinchang Wang & Wenxiao Huang & Snehashis Choudhury & Yu Zheng & Chibueze V. Amanchukwu & Samantha , 2020. "Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries," Nature Energy, Nature, vol. 5(7), pages 526-533, July.
  • Handle: RePEc:nat:natene:v:5:y:2020:i:7:d:10.1038_s41560-020-0634-5
    DOI: 10.1038/s41560-020-0634-5
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    Cited by:

    1. 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.
    2. 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.
    3. Shang Zhu & Bharath Ramsundar & Emil Annevelink & Hongyi Lin & Adarsh Dave & Pin-Wen Guan & Kevin Gering & Venkatasubramanian Viswanathan, 2024. "Differentiable modeling and optimization of non-aqueous Li-based battery electrolyte solutions using geometric deep learning," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. Chutao Wang & Zongqiang Sun & Yaqing Liu & Lin Liu & Xiaoting Yin & Qing Hou & Jingmin Fan & Jiawei Yan & Ruming Yuan & Mingsen Zheng & Quanfeng Dong, 2024. "A weakly coordinating-intervention strategy for modulating Na+ solvation sheathes and constructing robust interphase in sodium-metal batteries," Nature Communications, Nature, vol. 15(1), pages 1-14, 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. 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.
    7. 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.
    8. Mochou Liao & Xiao Ji & Yongjie Cao & Jie Xu & Xuan Qiu & Yihua Xie & Fei Wang & Chunsheng Wang & Yongyao Xia, 2022. "Solvent-free protic liquid enabling batteries operation at an ultra-wide temperature range," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    9. Yan Zhao & Tianhong Zhou & Timur Ashirov & Mario El Kazzi & Claudia Cancellieri & Lars P. H. Jeurgens & Jang Wook Choi & Ali Coskun, 2022. "Fluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    10. 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.
    11. 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.
    12. Yan Zhao & Tianhong Zhou & Mounir Mensi & Jang Wook Choi & Ali Coskun, 2023. "Electrolyte engineering via ether solvent fluorination for developing stable non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    13. Solomon T. Oyakhire & Wenbo Zhang & Andrew Shin & Rong Xu & David T. Boyle & Zhiao Yu & Yusheng Ye & Yufei Yang & James A. Raiford & William Huang & Joel R. Schneider & Yi Cui & Stacey F. Bent, 2022. "Electrical resistance of the current collector controls lithium morphology," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    14. Weili Zhang & Yang Lu & Lei Wan & Pan Zhou & Yingchun Xia & Shuaishuai Yan & Xiaoxia Chen & Hangyu Zhou & Hao Dong & Kai Liu, 2022. "Engineering a passivating electric double layer for high performance lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    15. Qing Zhao & Yue Deng & Nyalaliska W. Utomo & Jingxu Zheng & Prayag Biswal & Jiefu Yin & Lynden A. Archer, 2021. "On the crystallography and reversibility of lithium electrodeposits at ultrahigh capacity," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    16. 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.
    17. 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.
    18. Feifei Wang & Jipeng Zhang & Haotian Lu & Hanbing Zhu & Zihui Chen & Lu Wang & Jinyang Yu & Conghui You & Wenhao Li & Jianwei Song & Zhe Weng & Chunpeng Yang & Quan-Hong Yang, 2023. "Production of gas-releasing electrolyte-replenishing Ah-scale zinc metal pouch cells with aqueous gel electrolyte," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    19. 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.

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