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A locally solvent-tethered polymer electrolyte for long-life lithium metal batteries

Author

Listed:
  • Yanfei Zhu

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Zhoujie Lao

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Mengtian Zhang

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Tingzheng Hou

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Xiao Xiao

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Zhihong Piao

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Gongxun Lu

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Zhiyuan Han

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Runhua Gao

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Lu Nie

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Xinru Wu

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Yanze Song

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Chaoyuan Ji

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

  • Jian Wang

    (Canadian Light Source)

  • Guangmin Zhou

    (Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School)

Abstract

Solid polymer electrolytes exhibit enhanced Li+ conductivity when plasticized with highly dielectric solvents such as N,N-dimethylformamide (DMF). However, the application of DMF-containing electrolytes in solid-state batteries is hindered by poor cycle life caused by continuous DMF degradation at the anode surface and the resulting unstable solid-electrolyte interphase. Here we report a composite polymer electrolyte with a rationally designed Hofmann-DMF coordination complex to address this issue. DMF is engineered on Hofmann frameworks as tethered ligands to construct a locally DMF-rich interface which promotes Li+ conduction through a ligand-assisted transport mechanism. A high ionic conductivity of 6.5 × 10−4 S cm−1 is achieved at room temperature. We demonstrate that the composite electrolyte effectively reduces the free shuttling and subsequent decomposition of DMF. The locally solvent-tethered electrolyte cycles stably for over 6000 h at 0.1 mA cm−2 in Li | |Li symmetric cell. When paired with sulfurized polyacrylonitrile cathodes, the full cell exhibits a prolonged cycle life of 1000 cycles at 1 C. This work will facilitate the development of practical polymer-based electrolytes with high ionic conductivity and long cycle life.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48078-7
    DOI: 10.1038/s41467-024-48078-7
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    References listed on IDEAS

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    1. 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.
    2. Chunpeng Yang & Qisheng Wu & Weiqi Xie & Xin Zhang & Alexandra Brozena & Jin Zheng & Mounesha N. Garaga & Byung Hee Ko & Yimin Mao & Shuaiming He & Yue Gao & Pengbo Wang & Madhusudan Tyagi & Feng Jiao, 2021. "Copper-coordinated cellulose ion conductors for solid-state batteries," Nature, Nature, vol. 598(7882), pages 590-596, October.
    3. Michael J. Lee & Junghun Han & Kyungbin Lee & Young Jun Lee & Byoung Gak Kim & Kyu-Nam Jung & Bumjoon J. Kim & Seung Woo Lee, 2022. "Elastomeric electrolytes for high-energy solid-state lithium batteries," Nature, Nature, vol. 601(7892), pages 217-222, January.
    4. Xiulin Fan & Xiao Ji & Long Chen & Ji Chen & Tao Deng & Fudong Han & Jie Yue & Nan Piao & Ruixing Wang & Xiuquan Zhou & Xuezhang Xiao & Lixin Chen & Chunsheng Wang, 2019. "All-temperature batteries enabled by fluorinated electrolytes with non-polar solvents," Nature Energy, Nature, vol. 4(10), pages 882-890, October.
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