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ACS Publications. Most Trusted. Most Cited. Most Read
High-Voltage Potassium Hexacyanoferrate Cathode via High-Entropy and Potassium Incorporation for Stable Sodium-Ion Batteries
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    Article

    High-Voltage Potassium Hexacyanoferrate Cathode via High-Entropy and Potassium Incorporation for Stable Sodium-Ion Batteries
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    • Junyi Dai
      Junyi Dai
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      More by Junyi Dai
    • Sha Tan
      Sha Tan
      Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
      More by Sha Tan
    • Lifeng Wang
      Lifeng Wang
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      More by Lifeng Wang
    • Fangxin Ling
      Fangxin Ling
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      More by Fangxin Ling
    • Fuqiang Duan
      Fuqiang Duan
      College of Aerospace Science and Engineering, National University of Defense Technology, Chang Sha 410073, Hunan, China
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    • Mingze Ma
      Mingze Ma
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
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    • Yu Shao
      Yu Shao
      Jiujiang DeFu Technology Co., LTD., Jiujiang 332000, Jiangxi, China
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    • Xianhong Rui
      Xianhong Rui
      School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China
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    • Yu Yao
      Yu Yao
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      More by Yu Yao
    • Enyuan Hu
      Enyuan Hu
      Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
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    • Xiaojun Wu
      Xiaojun Wu
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
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    • Chunyang Li*
      Chunyang Li
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      *E-mail: [email protected]
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    • Yan Yu*
      Yan Yu
      Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, Anhui, China
      National Synchrotron Radiation Laboratory, Hefei, Anhui 230026, China
      *Email: [email protected]
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    Other Access OptionsSupporting Information (1)

    ACS Nano

    Cite this: ACS Nano 2023, 17, 21, 20949–20961
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    https://doi.org/10.1021/acsnano.3c02323
    Published October 31, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Prussian blue analogues (PBAs) used as sodium ion battery (SIB) cathodes are usually the focus of attention due to their three-dimensional open frame and high theoretical capacity. Nonetheless, the disadvantages of a low working voltage and inferior structural stability of PBAs prevent their further applications. Herein, we propose constructing the Kx(MnFeCoNiCu)[Fe(CN)6] (HE-K-PBA) cathode by high-entropy and potassium incorporation strategy to simultaneously realize high working voltage and cycling stability. The reaction mechanism of metal cations in HE-K-PBA are revealed by synchrotron radiation X-ray absorption spectroscopy (XAS), ex situ X-ray photoelectron spectroscopy (XPS), and in situ Raman spectra. We also investigate the entropy stabilization mechanism via finite element simulation, demonstrating that HE-K-PBA with small von Mises stress and weak structure strain can significantly mitigate the structural distortion. Benefit from the stable structure and everlasting K+ (de)intercalation, the HE-K-PBA delivers high output voltage (3.46 V), good reversible capacity (120.5 mAh g–1 at 0.01 A g–1), and capacity retention of 90.4% after 1700 cycles at 1.0 A g–1. Moreover, the assembled full cell and all-solid-state batteries with a stable median voltage of 3.29 V over 3000 cycles further demonstrate the application prospects of the HE-K-PBA cathode.

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    Supporting Information

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    . The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.3c02323.

    • Additional information and figures: detailed information about the XRD pattern; TEM image of Mn-K-PBA; HAADF STEM images, EDS mapping, XPS spectra, Raman spectra, TGA curves of HE-K-PBA and Mn-K-PBA; charge/discharge curves, CV curves, median voltages, Nyquist plots, comparison of normalized charge/discharge curves of HE-K-PBA and Mn-K-PBA; ex situ XRD, ex situ XPS analysis, ex situ TOF-SIMS analysis of HE-K-PBA and Mn-K-PBA; HAADF STEM images, energy dispersive X-ray spectroscopy, selected-area electron diffraction images, SEM images, and EDS mapping analysis of anodes; finite element simulation of Co-K-PBA, Ni-K-PBA, Cu-K-PBA and Fe-K-PBA (PDF)

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    Cited By

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    This article is cited by 2 publications.

    1. Xiaoying Zhao, Ningbo Liu, Mengxian Zheng, Xiaohan Wang, Yinuo Xu, Jingwei Liu, Fujun Li, Liubin Wang. Four-Electron Redox Reaction in Prussian Blue Analogue Cathode Material for High-Performance Sodium-Ion Batteries. ACS Energy Letters 2024, 9 (6) , 2748-2757. https://doi.org/10.1021/acsenergylett.4c00976
    2. Zinan Wang, Moulay Tahar Sougrati, Qiong Zheng, Rile Ge, Junhu Wang. Capacitive-Controlled Prussian White with a Nickel Iron Hexacyanoferrate Composite Cathode for Rapid Sodium Diffusion. ACS Applied Materials & Interfaces 2024, 16 (15) , 18908-18917. https://doi.org/10.1021/acsami.4c00885

    ACS Nano

    Cite this: ACS Nano 2023, 17, 21, 20949–20961
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.3c02323
    Published October 31, 2023
    Copyright © 2023 American Chemical Society

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