Achieving a high-performance sodium-ion pouch cell by regulating intergrowth structures in a layered oxide cathode with anionic redox

Xiaotong Wang, Qinghua Zhang, Chen Zhao, Haifeng Li, Baodan Zhang, Guifan Zeng, Yonglin Tang, Zhongyuan Huang, Inhui Hwang, Haitang Zhang, Shiyuan Zhou, Yongfu Qiu, Yinguo Xiao, Jordi Cabana, Cheng-Jun Sun, Khalil Amine, Yang Sun (), Qingsong Wang (), Gui-Liang Xu (), Lin Gu (), Yu Qiao () and Shi-Gang Sun
Additional contact information
Xiaotong Wang: Xiamen University
Qinghua Zhang: Chinese Academy of Sciences
Chen Zhao: Argonne National Laboratory
Haifeng Li: University of Illinois at Chicago
Baodan Zhang: Xiamen University
Guifan Zeng: Xiamen University
Yonglin Tang: Xiamen University
Zhongyuan Huang: Peking University
Inhui Hwang: Argonne National Laboratory
Haitang Zhang: Xiamen University
Shiyuan Zhou: Xiamen University
Yongfu Qiu: Dongguan University of Technology
Yinguo Xiao: Peking University
Jordi Cabana: University of Illinois at Chicago
Cheng-Jun Sun: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory
Yang Sun: Sun Yat-sen University
Qingsong Wang: University of Bayreuth
Gui-Liang Xu: Argonne National Laboratory
Lin Gu: Chinese Academy of Sciences
Yu Qiao: Xiamen University
Shi-Gang Sun: Xiamen University

Nature Energy, 2024, vol. 9, issue 2, 184-196

Abstract: Abstract In P2-type layered transition metal (TM) oxides, which are typical cathode materials for Na-ion batteries, the presence of Li within the TM layer could lead to the formation of specific Na–O–Li configurations that trigger additional oxygen redox at high charging voltages. However, the prismatic-type (P-type) to octahedral-type (O-type) phase transition and irreversible TM migration could be simultaneously aggravated in high state of charge, resulting in structural distortion. Here we demonstrate that excessive desodiation of P2-Na0.67Li0.1Fe0.37Mn0.53O2 (NLFMO) induces the formation of neighbouring O-type stacking faults with an intergrowth structure (that is, interlacing of O- and P-type layers), which leads to out-of-lattice Li migration and irreversible oxygen loss. We show that, by controlling the depth of charge to tailor the intergrowth structure, a P-type stacking state can be uniformly interspersed between the O-type stacking state, thereby avoiding neighbouring O-type stacking faults. Adjusting the O/P intergrowth structure leads to both reversible migration of Li/TM ions and reversible anionic redox in the NLFMO cathode. We thereby achieve a high-performance pouch cell (with an energy density of 165 W h kg−1 based on the entire weight of the cell) with both cationic and anionic redox activities.

Date: 2024
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DOI: 10.1038/s41560-023-01425-2

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