Reversible structural evolution of sodium-rich rhombohedral Prussian blue for sodium-ion batteries

Wanlin Wang, Yong Gang, Zhe Hu, Zichao Yan, Weijie Li, Yongcheng Li, Qin-Fen Gu (), Zhixing Wang, Shu-Lei Chou (), Hua-Kun Liu and Shi-Xue Dou
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Wanlin Wang: University of Wollongong, Innovation Campus, Squires Way
Yong Gang: Liaoning Starry Sky Sodium-ion Battery Co., Ltd., Laser industrial park, High-tech district
Zhe Hu: University of Wollongong, Innovation Campus, Squires Way
Zichao Yan: University of Wollongong, Innovation Campus, Squires Way
Weijie Li: University of Wollongong, Innovation Campus, Squires Way
Yongcheng Li: Liaoning Starry Sky Sodium-ion Battery Co., Ltd., Laser industrial park, High-tech district
Qin-Fen Gu: Australian Synchrotron (ANSTO), 800 Blackburn Road
Zhixing Wang: Central South University
Shu-Lei Chou: University of Wollongong, Innovation Campus, Squires Way
Hua-Kun Liu: University of Wollongong, Innovation Campus, Squires Way
Shi-Xue Dou: University of Wollongong, Innovation Campus, Squires Way

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Iron-based Prussian blue analogs are promising low-cost and easily prepared cathode materials for sodium-ion batteries. Their materials quality and electrochemical performance are heavily reliant on the precipitation process. Here we report a controllable precipitation method to synthesize high-performance Prussian blue for sodium-ion storage. Characterization of the nucleation and evolution processes of the highly crystalline Prussian blue microcubes reveals a rhombohedral structure that exhibits high initial Coulombic efficiency, excellent rate performance, and cycling properties. The phase transitions in the as-obtained material are investigated by synchrotron in situ powder X-ray diffraction, which shows highly reversible structural transformations between rhombohedral, cubic, and tetragonal structures upon sodium-ion (de)intercalations. Moreover, the Prussian blue material from a large-scale synthesis process shows stable cycling performance in a pouch full cell over 1000 times. We believe that this work could pave the way for the real application of Prussian blue materials in sodium-ion batteries.

Date: 2020
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DOI: 10.1038/s41467-020-14444-4

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