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Elucidation of the sodium kinetics in layered P-type oxide cathodes

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Abstract

Sodium-ion intercalation oxides generally possess high compositional diversity according to their different stacking sequences. The sodium diffusion pathway in layered P-type materials used in sodium-ion batteries is open, which can increase their rate capability by directly transmitting Na+ between adjacent triangular prismatic channels, rather than passing through an intermediate tetrahedral site in O-type structure. However, how the structure chemistry of the P-type oxides determines their electrochemical properties has not been fully understood yet. Herein, by comparing the crystalline structures, electrochemical behaviors, ion/electron transport dynamics of a couple of P-type intercalation cathodes, P2-Na2/3Ni1/3Mn2/3O2 and P3-Na2/3Ni1/3Mn2/3O2 with the same compositions, we demonstrate experimentally and computationally that the P2 phase delivers better cycling stability and rate capability than the P3 counterpart due to the predominant contribution of the faster intrinsic Na diffusion kinetics in the P2 bulk. We also point out that it is the electronic conductivity that captures the key electrochemistry of layered P3-type materials and makes them possible to enhance the sodium storage performance. The results reveal that the correlation between stacking structure and functional properties in two typical layered P-type cathodes, providing new guidelines for preparing and designing alkali-metal layered oxide materials with improved battery performance.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (U1607128, 52102302 and 21521005), Natural Science Foundation of Beijing (2222020), the Young Talent Support Plan and Siyuan Scholar of Xi’an Jiaotong University (DQ6J011 and DQ1J009), and State Key Laboratory of Electrical Insulation and Power Equipment (EIPE23313). The authors acknowledge the help from the Instrument Analysis Center and the High Performance Computing (HPC) Center at Xi’an Jiaotong University.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, China

    Lianzheng Yu, Yu-Xin Chang, Kang Xu & Sailong Xu

  2. Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi’an Jiaotong University, Xi’an, 710049, China

    Lianzheng Yu, Haojie Dong, Zhiwei Cheng, Yi-Hu Feng, Duo Si, Xu Zhu, Mengting Liu, Bing Xiao & Peng-Fei Wang

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  1. Lianzheng Yu
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Correspondence to Bing Xiao, Peng-Fei Wang or Sailong Xu.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Yu, L., Dong, H., Chang, YX. et al. Elucidation of the sodium kinetics in layered P-type oxide cathodes. Sci. China Chem. 65, 2005–2014 (2022). https://doi.org/10.1007/s11426-022-1364-1

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