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A stable cathode-solid electrolyte composite for high-voltage, long-cycle-life solid-state sodium-ion batteries

Author

Listed:
  • Erik A. Wu

    (University of California San Diego)

  • Swastika Banerjee

    (University of California San Diego)

  • Hanmei Tang

    (University of California San Diego)

  • Peter M. Richardson

    (University of California Santa Barbara)

  • Jean-Marie Doux

    (University of California San Diego)

  • Ji Qi

    (University of California San Diego)

  • Zhuoying Zhu

    (University of California San Diego)

  • Antonin Grenier

    (Stony Brook University)

  • Yixuan Li

    (University of California San Diego)

  • Enyue Zhao

    (University of California San Diego)

  • Grayson Deysher

    (University of California San Diego)

  • Elias Sebti

    (University of California Santa Barbara)

  • Han Nguyen

    (University of California San Diego)

  • Ryan Stephens

    (Shell International Exploration & Production Inc.)

  • Guy Verbist

    (Shell Global Solutions International BV)

  • Karena W. Chapman

    (Stony Brook University)

  • Raphaële J. Clément

    (University of California Santa Barbara)

  • Abhik Banerjee

    (University of California San Diego
    Research Institute for Sustainable Energy (RISE), TCG Centres for Research and Education in Science and Technology (TCG CREST))

  • Ying Shirley Meng

    (University of California San Diego
    University of California San Diego)

  • Shyue Ping Ong

    (University of California San Diego
    University of California San Diego)

Abstract

Rechargeable solid-state sodium-ion batteries (SSSBs) hold great promise for safer and more energy-dense energy storage. However, the poor electrochemical stability between current sulfide-based solid electrolytes and high-voltage oxide cathodes has limited their long-term cycling performance and practicality. Here, we report the discovery of the ion conductor Na3-xY1-xZrxCl6 (NYZC) that is both electrochemically stable (up to 3.8 V vs. Na/Na+) and chemically compatible with oxide cathodes. Its high ionic conductivity of 6.6 × 10−5 S cm−1 at ambient temperature, several orders of magnitude higher than oxide coatings, is attributed to abundant Na vacancies and cooperative MCl6 rotation, resulting in an extremely low interfacial impedance. A SSSB comprising a NaCrO2 + NYZC composite cathode, Na3PS4 electrolyte, and Na-Sn anode exhibits an exceptional first-cycle Coulombic efficiency of 97.1% at room temperature and can cycle over 1000 cycles with 89.3% capacity retention at 40 °C. These findings highlight the immense potential of halides for SSSB applications.

Suggested Citation

  • Erik A. Wu & Swastika Banerjee & Hanmei Tang & Peter M. Richardson & Jean-Marie Doux & Ji Qi & Zhuoying Zhu & Antonin Grenier & Yixuan Li & Enyue Zhao & Grayson Deysher & Elias Sebti & Han Nguyen & Ry, 2021. "A stable cathode-solid electrolyte composite for high-voltage, long-cycle-life solid-state sodium-ion batteries," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21488-7
    DOI: 10.1038/s41467-021-21488-7
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    Cited by:

    1. Ge Sun & Chenjie Lou & Boqian Yi & Wanqing Jia & Zhixuan Wei & Shiyu Yao & Ziheng Lu & Gang Chen & Zexiang Shen & Mingxue Tang & Fei Du, 2023. "Electrochemically induced crystalline-to-amorphization transformation in sodium samarium silicate solid electrolyte for long-lasting sodium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Hong Fang & Puru Jena, 2022. "Argyrodite-type advanced lithium conductors and transport mechanisms beyond paddle-wheel effect," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Tom Lee & Ji Qi & Chaitanya A. Gadre & Huaixun Huyan & Shu-Ting Ko & Yunxing Zuo & Chaojie Du & Jie Li & Toshihiro Aoki & Ruqian Wu & Jian Luo & Shyue Ping Ong & Xiaoqing Pan, 2023. "Atomic-scale origin of the low grain-boundary resistance in perovskite solid electrolyte Li0.375Sr0.4375Ta0.75Zr0.25O3," 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. Hiram Kwak & Jae-Seung Kim & Daseul Han & Jong Seok Kim & Juhyoun Park & Gihan Kwon & Seong-Min Bak & Unseon Heo & Changhyun Park & Hyun-Wook Lee & Kyung-Wan Nam & Dong-Hwa Seo & Yoon Seok Jung, 2023. "Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries," Nature Communications, Nature, vol. 14(1), pages 1-14, December.

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