Tuning cyanide coordination electronic structure enables stable Prussian blue analogues for sodium-ion batteries

Yuanheng Wang, Jiaxin Yan, Bingxing Xie (), Yan Meng, Chuankai Fu, Fanpeng Kong, Xingyu Wang, Qingjie Zhou, Xin Chen, Jianting Li, Chunyu Du, Liguang Wang () and Pengjian Zuo ()
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Yuanheng Wang: Harbin Institute of Technology
Jiaxin Yan: Harbin Institute of Technology
Bingxing Xie: Nanjing University of Science and Technology
Yan Meng: Harbin Institute of Technology
Chuankai Fu: Harbin Institute of Technology
Fanpeng Kong: Harbin Institute of Technology
Xingyu Wang: Harbin Institute of Technology
Qingjie Zhou: Harbin Institute of Technology
Xin Chen: Harbin Institute of Technology
Jianting Li: Harbin Institute of Technology
Chunyu Du: Harbin Institute of Technology
Liguang Wang: Zhejiang University
Pengjian Zuo: Harbin Institute of Technology

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Prussian blue analogues exhibit significant potential as positive electrode materials for sodium-ion batteries, particularly due to their three-dimensional cyanide-bridged frameworks which facilitate fast charging capabilities. However, the labile chemical bonds coordinated by transition metal ions and cyanide ligands often lead to structural instability, causing serious electrochemical degradations during cycling. Fundamentally understanding and controlling the local electronic structure to mitigate this instability remains challenging. Herein, we approach this problem by modulating the local electronic structure surrounding nitrogen-coordinated transition metal ions to create a uniform electron distribution within the Prussian blue analogues frameworks. The resulting uniform electronic structure enhances the reactivity of both nitrogen-coordinated and carbon-coordinated transition metals. More importantly, the reduction of electronic displacement through regulated coordination significantly improves the crystal structural stability, yielding a capacity retention of over 91% at 5 C after 1000 cycles. These findings provide insights into the local structural chemistry of Prussian blue analogues and offer guidance for the development of positive materials for sodium-ion batteries.

Date: 2025
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DOI: 10.1038/s41467-025-65062-x

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