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Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries

Author

Listed:
  • Fang Fu

    (College of Materials Science and Engineering, Huaqiao University)

  • Xiang Liu

    (Argonne National Laboratory)

  • Xiaoguang Fu

    (College of Materials Science and Engineering, Huaqiao University)

  • Hongwei Chen

    (College of Materials Science and Engineering, Huaqiao University)

  • Ling Huang

    (College of Chemistry and Chemical Engineering, Xiamen University)

  • Jingjing Fan

    (College of Chemistry and Chemical Engineering, Xiamen University)

  • Jiabo Le

    (College of Chemistry and Chemical Engineering, Xiamen University)

  • Qiuxiang Wang

    (College of Materials Science and Engineering, Huaqiao University)

  • Weihua Yang

    (College of Materials Science and Engineering, Huaqiao University)

  • Yang Ren

    (Advanced Photon Source, Argonne National Laboratory)

  • Khalil Amine

    (Argonne National Laboratory
    Materials Science and Engineering, Stanford University
    Materials Science and Nano-engineering, Mohammed VI Polytechnic University)

  • Shi-Gang Sun

    (College of Chemistry and Chemical Engineering, Xiamen University)

  • Gui-Liang Xu

    (Argonne National Laboratory)

Abstract

P2-type sodium manganese-rich layered oxides are promising cathode candidates for sodium-based batteries because of their appealing cost-effective and capacity features. However, the structural distortion and cationic rearrangement induced by irreversible phase transition and anionic redox reaction at high cell voltage (i.e., >4.0 V) cause sluggish Na-ion kinetics and severe capacity decay. To circumvent these issues, here, we report a strategy to develop P2-type layered cathodes via configurational entropy and ion-diffusion structural tuning. In situ synchrotron X-ray diffraction combined with electrochemical kinetic tests and microstructural characterizations reveal that the entropy-tuned Na0.62Mn0.67Ni0.23Cu0.05Mg0.07Ti0.01O2 (CuMgTi-571) cathode possesses more {010} active facet, improved structural and thermal stability and faster anionic redox kinetics compared to Na0.62Mn0.67Ni0.37O2. When tested in combination with a Na metal anode and a non-aqueous NaClO4-based electrolyte solution in coin cell configuration, the CuMgTi-571-based positive electrode enables an 87% capacity retention after 500 cycles at 120 mA g−1 and about 75% capacity retention after 2000 cycles at 1.2 A g−1.

Suggested Citation

  • Fang Fu & Xiang Liu & Xiaoguang Fu & Hongwei Chen & Ling Huang & Jingjing Fan & Jiabo Le & Qiuxiang Wang & Weihua Yang & Yang Ren & Khalil Amine & Shi-Gang Sun & Gui-Liang Xu, 2022. "Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30113-0
    DOI: 10.1038/s41467-022-30113-0
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    References listed on IDEAS

    as
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    1. Jiyu Zhang & Yongliang Yan & Xin Wang & Yanyan Cui & Zhengfeng Zhang & Sen Wang & Zhengkun Xie & Pengfei Yan & Weihua Chen, 2023. "Bridging multiscale interfaces for developing ionically conductive high-voltage iron sulfate-containing sodium-based battery positive electrodes," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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