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Understanding capacity fading from structural degradation in Prussian blue analogues for wide-temperature sodium-ion cylindrical battery

Hang Zhang, Jiayang Li, Jinhang Liu, Yun Gao (), Yameng Fan, Xiaohao Liu, Chaofei Guo, Haoxuan Liu, Xiudong Chen (), Xingqiao Wu, Yang Liu, Qinfen Gu, Li Li (), Jiazhao Wang and Shu-Lei Chou ()
Additional contact information
Hang Zhang: Wenzhou University
Jiayang Li: Squires Way
Jinhang Liu: Jiujiang University
Yun Gao: Wenzhou University
Yameng Fan: Squires Way
Xiaohao Liu: Wenzhou University
Chaofei Guo: Shanghai University
Haoxuan Liu: Squires Way
Xiudong Chen: Jiujiang University
Xingqiao Wu: Wenzhou University
Yang Liu: Shanghai University
Qinfen Gu: Australian Synchrotron (ANSTO) 800 Blackburn Road
Li Li: Shanghai University
Jiazhao Wang: Wenzhou University
Shu-Lei Chou: Wenzhou University

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Low-cost Fe-based Prussian blue analogues often suffer from capacity degradation, resulting in continuous energy loss, impeding commercialization for practical sodium-ion batteries. The underlying cause of capacity decrease remains mysterious. Herein, we show that irreversible phase transitions, structural degradation, deactivation of surface redox centres, and dissolution of transition metal ions in Prussian blue analogues accumulate continuously during cycling. These undesirable changes are responsible for massive destruction of their morphology, leading to the capacity decay. A dual regulation strategy is applied to alleviate the above-mentioned problems of Prussian blue analogues. The designed 18650/33140 cylindrical cells using modified Prussian blue analogues and hard carbon display improved cycling stability and wide-temperature working performance (−40 oC–100 oC). The findings resolve the controversy over the origins of Prussian blue analogues cathode degradation, emphasize the necessity of eliminating irreversible crystal/structural changes to guarantee enhanced cycling stability, and demonstrate the potential of Prussian blue analogues cathode for commercial sodium-ion batteries.

Date: 2025
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DOI: 10.1038/s41467-025-57663-3

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