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Zhang et al. Energy Mater 2023;3:300008 Energy Materials
DOI: 10.20517/energymater.2022.71

Article Open Access

Enhanced all-climate sodium-ion batteries

performance in a low-defect and Na-enriched
Prussian blue analogue cathode by nickel

substitution

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Jingwen Zhang , Jing Wan , Mingyang Ou , Siying Liu , Bicheng Huang , Jia Xu , Shixiong Sun , Yue Xu ,
1,
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Yaqing Lin *, Chun Fang *, Jiantao Han 1
1
State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering,
Huazhong University of Science and Technology, Wuhan 430074, Hubei, China.
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Department of Applied Physics, Chongqing University, Chongqing 401331, China.
* Correspondence to: Yaqing Lin, State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials
Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China. E-mail:
359702366@qq.com; Dr. Assoc. Prof. Chun Fang, a State Key Laboratory of Material Processing and Die & Mould Technology,
School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China.
E-mail: fangchun@hust.edu.cn
How to cite this article: Zhang J, Wan J, Ou M, Liu S, Huang B, Xu J, Sun S, Xu Y, Lin Y, Fang C, Han J. Enhanced all-climate
sodium-ion batteries performance in a low-defect and Na-enriched Prussian blue analogue cathode by nickel substitution. Energy
Mater 2023;3:300008. https://dx.doi.org/10.20517/energymater.2022.71
Received: 31 Oct 2022 First Decision: 5 Dec 2022 Revised: 26 Dec 2022 Accepted: 19 Jan 2023 Published: 14 Feb 2023
Academic Editors: Yuping Wu, Jiazhao Wang Copy Editor: Fangling Lan Production Editor: Fangling Lan

Abstract
Cobalt hexacyanoferrate (CoHCF) is one of the most promising cathode materials for all-climate sodium-ion
batteries (SIBs) due to its open three-dimensional (3D) framework structures, high theoretical specific capacity,
good voltage platform and almost no Jahn-Teller effects. However, CoHCF still suffers from poor cycling stability
and bad rate capability, which is closely related to the huge distortion of frame structure and poor conductivity. In
this study, by choosing nickel (Ni) to partially replace cobalt (Co) in the CoHCF lattice, we successfully prepared
low-defect and Na-enriched Na Co Ni [Fe(CN) ] (Co Ni HCF) in chelate and sodium salt-assisted
0.7
2
0.7
0.3
6
0.3
coprecipitation method. Both experiments and first-principles calculations demonstrate that Ni substitution can
effectively suppress the lattice distortion during the charging and discharging process of CoHCF. Furthermore, the
introduction of Ni increases ion mobility by reducing the ion migration barrier (0.31 eV versus 0.17 eV) and
improves the electronic conductivity by reducing the bandgap. It is found that Co Ni HCF exhibits superior
0.7
0.3
electrochemical performance compared with that of CoHCF in a wide temperature range (-30 to 60 °C). At 25 °C,
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