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Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes

Author

Listed:
  • Zeyu Deng

    (National University of Singapore)

  • Tara P. Mishra

    (National University of Singapore
    Singapore-MIT Alliance for Research and Technology)

  • Eunike Mahayoni

    (Laboratoire de Réactivité et de Chimie des Solides (LRCS), CNRS UMR 7314, Université de Picardie Jules Verne
    RS2E, Réseau Français sur le Stockage Electrochimique de l’Energie, FR CNRS 3459
    ALISTORE-ERI European Research Institute, FR CNRS 3104)

  • Qianli Ma

    (Materials Synthesis and Processing (IEK-1))

  • Aaron Jue Kang Tieu

    (National University of Singapore)

  • Olivier Guillon

    (Materials Synthesis and Processing (IEK-1)
    Helmholtz-Institute Münster, c/o Forschungszentrum Jülich GmbH)

  • Jean-Noël Chotard

    (Laboratoire de Réactivité et de Chimie des Solides (LRCS), CNRS UMR 7314, Université de Picardie Jules Verne
    RS2E, Réseau Français sur le Stockage Electrochimique de l’Energie, FR CNRS 3459
    ALISTORE-ERI European Research Institute, FR CNRS 3104)

  • Vincent Seznec

    (Laboratoire de Réactivité et de Chimie des Solides (LRCS), CNRS UMR 7314, Université de Picardie Jules Verne
    RS2E, Réseau Français sur le Stockage Electrochimique de l’Energie, FR CNRS 3459
    ALISTORE-ERI European Research Institute, FR CNRS 3104)

  • Anthony K. Cheetham

    (National University of Singapore
    University of California)

  • Christian Masquelier

    (Laboratoire de Réactivité et de Chimie des Solides (LRCS), CNRS UMR 7314, Université de Picardie Jules Verne
    RS2E, Réseau Français sur le Stockage Electrochimique de l’Energie, FR CNRS 3459
    ALISTORE-ERI European Research Institute, FR CNRS 3104)

  • Gopalakrishnan Sai Gautam

    (Indian Institute of Science)

  • Pieremanuele Canepa

    (National University of Singapore
    Singapore-MIT Alliance for Research and Technology
    National University of Singapore)

Abstract

Lithium and sodium (Na) mixed polyanion solid electrolytes for all-solid-state batteries display some of the highest ionic conductivities reported to date. However, the effect of polyanion mixing on the ion-transport properties is still not fully understood. Here, we focus on Na1+xZr2SixP3−xO12 (0 ≤ x ≤ 3) NASICON electrolyte to elucidate the role of polyanion mixing on the Na-ion transport properties. Although NASICON is a widely investigated system, transport properties derived from experiments or theory vary by orders of magnitude. We use more than 2000 distinct ab initio-based kinetic Monte Carlo simulations to map the compositional space of NASICON over various time ranges, spatial resolutions and temperatures. Via electrochemical impedance spectroscopy measurements on samples with different sodium content, we find that the highest ionic conductivity (i.e., about 0.165 S cm–1 at 473 K) is experimentally achieved in Na3.4Zr2Si2.4P0.6O12, in line with simulations (i.e., about 0.170 S cm–1 at 473 K). The theoretical studies indicate that doped NASICON compounds (especially those with a silicon content x ≥ 2.4) can improve the Na-ion mobility compared to undoped NASICON compositions.

Suggested Citation

  • Zeyu Deng & Tara P. Mishra & Eunike Mahayoni & Qianli Ma & Aaron Jue Kang Tieu & Olivier Guillon & Jean-Noël Chotard & Vincent Seznec & Anthony K. Cheetham & Christian Masquelier & Gopalakrishnan Sai , 2022. "Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32190-7
    DOI: 10.1038/s41467-022-32190-7
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    References listed on IDEAS

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    1. Bin Ouyang & Jingyang Wang & Tanjin He & Christopher J. Bartel & Haoyan Huo & Yan Wang & Valentina Lacivita & Haegyeom Kim & Gerbrand Ceder, 2021. "Synthetic accessibility and stability rules of NASICONs," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Xingfeng He & Yizhou Zhu & Yifei Mo, 2017. "Origin of fast ion diffusion in super-ionic conductors," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
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    Cited by:

    1. Chengyu Fu & Yifan Li & Wenjie Xu & Xuyong Feng & Weijian Gu & Jue Liu & Wenwen Deng & Wei Wang & A. M. Milinda Abeykoon & Laisuo Su & Lingyun Zhu & Xiaojun Wu & Hongfa Xiang, 2024. "LaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Jingyang Wang & Tanjin He & Xiaochen Yang & Zijian Cai & Yan Wang & Valentina Lacivita & Haegyeom Kim & Bin Ouyang & Gerbrand Ceder, 2023. "Design principles for NASICON super-ionic conductors," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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