Tailoring planar strain for robust structural stability in high-entropy layered sodium oxide cathode materials

Feixiang Ding, Pengxiang Ji, Zhen Han, Xueyan Hou, Yang Yang, Zilin Hu, Yaoshen Niu, Yuan Liu, Jiao Zhang, Xiaohui Rong, Yaxiang Lu (), Huican Mao (), Dong Su (), Liquan Chen and Yong-Sheng Hu ()
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Feixiang Ding: Chinese Academy of Sciences
Pengxiang Ji: Chinese Academy of Sciences
Zhen Han: Chinese Academy of Sciences
Xueyan Hou: Chinese Academy of Sciences
Yang Yang: Chinese Academy of Sciences
Zilin Hu: Chinese Academy of Sciences
Yaoshen Niu: Chinese Academy of Sciences
Yuan Liu: Chinese Academy of Sciences
Jiao Zhang: Chinese Academy of Sciences
Xiaohui Rong: Chinese Academy of Sciences
Yaxiang Lu: Chinese Academy of Sciences
Huican Mao: University of Science and Technology Beijing
Dong Su: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences
Yong-Sheng Hu: Chinese Academy of Sciences

Nature Energy, 2024, vol. 9, issue 12, 1529-1539

Abstract: Abstract High-entropy oxides have expanded the potential for high-performance Na-ion battery cathodes due to their vast compositional space and entropy-driven stabilization. However, a rational design approach for optimizing their composition is still lacking. Here, we develop an O3-type oxide cathode composed of all-3d transition metals, NaNi0.3Cu0.1Fe0.2Mn0.3Ti0.1O2 (NCFMT), which exhibits improved reversible specific capacity and exceptional cycling stability. Replacing Ti4+ with Sn4+ ions (NaNi0.3Cu0.1Fe0.2Mn0.3Sn0.1O2; NCFMS) results in poor structural reversibility and diminished cycling stability. Our investigations suggest that the structural integrity of the layered cathode is affected by the compatibility of constituent elements within the transition metal layers (TMO2). In NCFMS, planar strain induced by metal-ion displacement triggers elemental segregation and crack formation during repeated cycling. In contrast, NCFMT demonstrates a robust structural framework for stable Na+ storage due to its high mechanochemical compatibility among constituent elements. This understanding provides insights for designing outstanding layered high-entropy cathode materials.

Date: 2024
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DOI: 10.1038/s41560-024-01616-5

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