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

Fang Fu (fufang@hqu.edu.cn), Xiang Liu, Xiaoguang Fu, Hongwei Chen, Ling Huang, Jingjing Fan, Jiabo Le, Qiuxiang Wang, Weihua Yang, Yang Ren, Khalil Amine (amine@anl.gov), Shi-Gang Sun (sgsun@xmu.edu.cn) and Gui-Liang Xu (xug@anl.gov)
Additional contact information
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
Shi-Gang Sun: College of Chemistry and Chemical Engineering, Xiamen University
Gui-Liang Xu: Argonne National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-30113-0

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