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

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...

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Main Authors: 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, Yong-Sheng Hu
Format: Article
Language:English
Published: Nature Portfolio 2025-05-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-59980-z
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author 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
Yong-Sheng Hu
author_facet 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
Yong-Sheng Hu
author_sort Qiubo Guo
collection DOAJ
description 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.
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spelling doaj-art-e9c6490a2eb047408d81c5ce383e1b142025-08-20T03:48:19ZengNature PortfolioNature Communications2041-17232025-05-0116111310.1038/s41467-025-59980-zCation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteriesQiubo Guo0Shuai Han1Yaxiang Lu2Ruijuan Xiao3Jin Li4Qingli Hao5Xiaohui Rong6Suting Weng7Yaoshen Niu8Feixiang Ding9Yang Yang10Hui Xia11Xuefeng Wang12Fei Xie13Lin Zhou14Xueyan Hou15Hong Li16Xuejie Huang17Liquan Chen18Yong-Sheng Hu19Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesHerbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and TechnologyKey Laboratory for Soft Chemistry and Functional Materials, Ministry of Education, School of Chemical Engineering, Nanjing University of Science and TechnologyKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesHerbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and TechnologyKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesKey Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of SciencesAbstract 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.https://doi.org/10.1038/s41467-025-59980-z
spellingShingle 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
Yong-Sheng Hu
Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
Nature Communications
title Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
title_full Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
title_fullStr Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
title_full_unstemmed Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
title_short Cation-self-shielding strategy promises high-voltage all-Prussian-blue-based aqueous K-ion batteries
title_sort cation self shielding strategy promises high voltage all prussian blue based aqueous k ion batteries
url https://doi.org/10.1038/s41467-025-59980-z
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