Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries

Qiubo Guo, Shuai Han, Yaxiang Lu (), Ruijuan Xiao (), Jin Li, Qingli Hao, Xiaohui Rong, Suting Weng, Yaoshen Niu, Feixiang Ding, Yang Yang, Hui Xia, Xuefeng Wang, Fei Xie, Lin Zhou, Xueyan Hou, Hong Li, Xuejie Huang, Liquan Chen and Yong-Sheng Hu ()
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Qiubo Guo: Chinese Academy of Sciences
Shuai Han: Chinese Academy of Sciences
Yaxiang Lu: Chinese Academy of Sciences
Ruijuan Xiao: Chinese Academy of Sciences
Jin Li: Nanjing University of Science and Technology
Qingli Hao: Nanjing University of Science and Technology
Xiaohui Rong: Chinese Academy of Sciences
Suting Weng: Chinese Academy of Sciences
Yaoshen Niu: Chinese Academy of Sciences
Feixiang Ding: Chinese Academy of Sciences
Yang Yang: Chinese Academy of Sciences
Hui Xia: Nanjing University of Science and Technology
Xuefeng Wang: Chinese Academy of Sciences
Fei Xie: Chinese Academy of Sciences
Lin Zhou: Chinese Academy of Sciences
Xueyan Hou: Chinese Academy of Sciences
Hong Li: Chinese Academy of Sciences
Xuejie Huang: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences
Yong-Sheng Hu: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Prussian blue analogues (PBAs) are promising electrode candidates for aqueous batteries because the inevitable interstitial water is generally thought to have little impact on battery performance. Currently, mounting researches have focused on optimizing PBA properties by varying transition metal composition, but less attention has been paid to interstitial water, especially in alkali metal-ion deficient PBAs with large cavities. Here, we employ the water-rich K0.01Mn[Cr(CN)6]0.74·4.75H2O as the negative electrode to study the effect of interstitial water. It is found that during de-potassiation, the electrode undergoes dehydration, which negatively impacts kinetics, distorts structure, and raises charging potential. A cation-self-shielding strategy involving Dihydroxyacetone (DHA) in the electrolyte to secure the water-rich state is then proposed. The built 1.82 V all-Prussian blue aqueous K-ion battery delivers a high practical specific energy of ~76 Wh kg−1 over 1.5 V (based on the total mass of active materials in both electrodes). This study reveals the significance of interstitial water on the kinetics of PBA negative electrodes and promotes the exploration of water-containing electrodes to develop high-voltage aqueous rechargeable batteries for energy storage applications.

Date: 2025
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DOI: 10.1038/s41467-025-59980-z

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