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Slight compositional variation-induced structural disorder-to-order transition enables fast Na+ storage in layered transition metal oxides

Author

Listed:
  • Yuansheng Shi

    (Sun Yat-sen University)

  • Pengfeng Jiang

    (Sun Yat-sen University)

  • Shicheng Wang

    (Sun Yat-sen University)

  • Weixin Chen

    (Sun Yat-sen University)

  • Bin Wei

    (Sun Yat-sen University)

  • Xueyi Lu

    (Sun Yat-sen University)

  • Guoyu Qian

    (Sun Yat-sen University)

  • Wang Hay Kan

    (Spallation Neutron Source Science Center
    Chinese Academy of Sciences)

  • Huaican Chen

    (Spallation Neutron Source Science Center
    Chinese Academy of Sciences)

  • Wen Yin

    (Spallation Neutron Source Science Center
    Chinese Academy of Sciences)

  • Yang Sun

    (Sun Yat-sen University)

  • Xia Lu

    (Sun Yat-sen University)

Abstract

The omnipresent Na+/vacancy orderings change substantially with the composition that inevitably actuate the ionic diffusion in rechargeable batteries. Therefore, it may hold the key to the electrode design with high rate capability. Herein, the influence of Na+/vacancy ordering on Na+ mobility is demonstrated firstly through a comparative investigation in P2-Na2/3Ni1/3Mn2/3O2 and P2-Na2/3Ni0.3Mn0.7O2. The large zigzag Na+/vacancy intralayer ordering is found to accelerate Na+ migration in P2-type Na2/3Ni1/3Mn2/3O2. By theoretical simulations, it is revealed that the Na+ ordering enables the P2-type Na2/3Ni1/3Mn2/3O2 with higher diffusivities and lower activation energies of 200 meV with respect to the P3 one. The quantifying diffusional analysis further prove that the higher probability of the concerted Na+ ionic diffusion occurs in P2-type Na2/3Ni1/3Mn2/3O2 due to the appropriate ratio of high energy ordered Na ions (Naf) occupation. As a result, the interplay between the Na+/vacancy ordering and Na+ kinetic is well understood in P2-type layered cathodes.

Suggested Citation

  • Yuansheng Shi & Pengfeng Jiang & Shicheng Wang & Weixin Chen & Bin Wei & Xueyi Lu & Guoyu Qian & Wang Hay Kan & Huaican Chen & Wen Yin & Yang Sun & Xia Lu, 2022. "Slight compositional variation-induced structural disorder-to-order transition enables fast Na+ storage in layered transition metal oxides," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35597-4
    DOI: 10.1038/s41467-022-35597-4
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