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Copper-coordinated cellulose ion conductors for solid-state batteries

Author

Listed:
  • Chunpeng Yang

    (University of Maryland)

  • Qisheng Wu

    (Brown University)

  • Weiqi Xie

    (University of Maryland)

  • Xin Zhang

    (University of Maryland)

  • Alexandra Brozena

    (University of Maryland)

  • Jin Zheng

    (Florida State University)

  • Mounesha N. Garaga

    (City University of New York)

  • Byung Hee Ko

    (University of Delaware)

  • Yimin Mao

    (University of Maryland
    National Institute of Standards and Technology (NIST))

  • Shuaiming He

    (University of Maryland)

  • Yue Gao

    (University of Maryland)

  • Pengbo Wang

    (Florida State University)

  • Madhusudan Tyagi

    (University of Maryland
    National Institute of Standards and Technology (NIST))

  • Feng Jiao

    (University of Delaware)

  • Robert Briber

    (University of Maryland)

  • Paul Albertus

    (University of Maryland)

  • Chunsheng Wang

    (University of Maryland)

  • Steven Greenbaum

    (City University of New York)

  • Yan-Yan Hu

    (Florida State University
    National High Magnetic Field Laboratory)

  • Akira Isogai

    (The University of Tokyo)

  • Martin Winter

    (Institute of Physical Chemistry, University of Münster)

  • Kang Xu

    (Army Research Laboratory)

  • Yue Qi

    (Brown University)

  • Liangbing Hu

    (University of Maryland
    University of Maryland)

Abstract

Although solid-state lithium (Li)-metal batteries promise both high energy density and safety, existing solid ion conductors fail to satisfy the rigorous requirements of battery operations. Inorganic ion conductors allow fast ion transport, but their rigid and brittle nature prevents good interfacial contact with electrodes. Conversely, polymer ion conductors that are Li-metal-stable usually provide better interfacial compatibility and mechanical tolerance, but typically suffer from inferior ionic conductivity owing to the coupling of the ion transport with the motion of the polymer chains1–3. Here we report a general strategy for achieving high-performance solid polymer ion conductors by engineering of molecular channels. Through the coordination of copper ions (Cu2+) with one-dimensional cellulose nanofibrils, we show that the opening of molecular channels within the normally ion-insulating cellulose enables rapid transport of Li+ ions along the polymer chains. In addition to high Li+ conductivity (1.5 × 10−3 siemens per centimetre at room temperature along the molecular chain direction), the Cu2+-coordinated cellulose ion conductor also exhibits a high transference number (0.78, compared with 0.2–0.5 in other polymers2) and a wide window of electrochemical stability (0–4.5 volts) that can accommodate both the Li-metal anode and high-voltage cathodes. This one-dimensional ion conductor also allows ion percolation in thick LiFePO4 solid-state cathodes for application in batteries with a high energy density. Furthermore, we have verified the universality of this molecular-channel engineering approach with other polymers and cations, achieving similarly high conductivities, with implications that could go beyond safe, high-performance solid-state batteries.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:nature:v:598:y:2021:i:7882:d:10.1038_s41586-021-03885-6
    DOI: 10.1038/s41586-021-03885-6
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    Citations

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    Cited by:

    1. Kai Li & Jifeng Wang & Yuanyuan Song & Ying Wang, 2023. "Machine learning-guided discovery of ionic polymer electrolytes for lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Chao Chen & Jiaming Zhang & Benrui Hu & Qianwen Liang & Xunhui Xiong, 2023. "Dynamic gel as artificial interphase layer for ultrahigh-rate and large-capacity lithium metal anode," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. 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.
    4. Davood Sabaghi & Zhiyong Wang & Preeti Bhauriyal & Qiongqiong Lu & Ahiud Morag & Daria Mikhailovia & Payam Hashemi & Dongqi Li & Christof Neumann & Zhongquan Liao & Anna Maria Dominic & Ali Shaygan Ni, 2023. "Ultrathin positively charged electrode skin for durable anion-intercalation battery chemistries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Xiansheng Zhang & Hongwei Yan & Chongzhi Xu & Xia Dong & Yu Wang & Aiping Fu & Hao Li & Jin Yong Lee & Sheng Zhang & Jiahua Ni & Min Gao & Jing Wang & Jinpeng Yu & Shuzhi Sam Ge & Ming Liang Jin & Lil, 2023. "Skin-like cryogel electronics from suppressed-freezing tuned polymer amorphization," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Hanwen An & Menglu Li & Qingsong Liu & Yajie Song & Jiaxuan Liu & Zhihang Yu & Xingjiang Liu & Biao Deng & Jiajun Wang, 2024. "Strong Lewis-acid coordinated PEO electrolyte achieves 4.8 V-class all-solid-state batteries over 580 Wh kg−1," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    7. 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.
    8. Qinglu Liu & Tang Tang & Ziyu Tian & Shiwen Ding & Linqin Wang & Dexin Chen & Zhiwei Wang & Wentao Zheng & Husileng Lee & Xingyu Lu & Xiaohe Miao & Lin Liu & Licheng Sun, 2024. "A high-performance watermelon skin ion-solvating membrane for electrochemical CO2 reduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    9. Linyi Zhao & Tiansheng Wang & Fengkai Zuo & Zhengyu Ju & Yuhao Li & Qiang Li & Yue Zhu & Hongsen Li & Guihua Yu, 2024. "A fast-charging/discharging and long-term stable artificial electrode enabled by space charge storage mechanism," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    10. Jine Wu & Chenyi Liao & Tianyu Li & Jing Zhou & Linjuan Zhang & Jian-Qiang Wang & Guohui Li & Xianfeng Li, 2023. "Metal-coordinated polybenzimidazole membranes with preferential K+ transport," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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