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Boosting the sodium storage performance of Prussian blue analogues via effective etching

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Abstract

Prussian blue analogues (PBAs) have gained significant popularity as cathode materials for sodium-ion batteries (SIBs) due to their remarkable features such as high capacity and convenient synthesis. However, PBAs usually suffer from kinetic problems during the electrochemical reactions due to sluggish Na+ diffusion in the large crystals, resulting in low-capacity utilization and inferior rate capability. In this study, we present a facile etching method aiming at activating the sodium storage sites and accelerating the Na+ transport of Na2NiFe(CN)6 (denoted as NaNiHCF) by precisely controlling its morphologies. A progressive corner passivation phenomenon occurred in NaNiHCF during the etching process, which led to a substantial augmentation of the specific surface area as the morphology transitioned from a standard cube to a dice shape. Notably, by controlling the etching time, the obtained NaNiHCF-3 electrode exhibited boosted electrochemical performance with high reversible capacity of 83.5 mAh g−1 (98.2% of its theoretical capacity), superior rate capability (71.2 mAh g−1 at 10 C), and stable cycling life-span at different temperatures. Both experimental and computational methods reveal the remarkably reversible structural evolution process and improved Na+ diffusion coefficient. We believe that this work can serve as an indispensable reference to tailor the structure of PBAs to obtain improved electrochemical performance.

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Acknowledgements This work is financially supported from the National Natural Science Foundation of China (U20A20249, 21972108, and 22209125). The numerical calculations in this paper have been done on the supercomputing system in the Supercomputing Center of Wuhan University.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China

    Yanan Zhao, Kean Chen, Laibing Luo, Hui Chen, Xinping Ai, Yongjin Fang & Yuliang Cao

  2. Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Innovation Campus, Squires Way, North Wollongong, 2522, Australia

    Jian Peng, Hang Zhang & Shulei Chou

  3. Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, China

    Shulei Chou

  4. College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Xiangmin Feng, Weihua Chen & Ruoyu Cao

Authors
  1. Yanan Zhao
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  2. Jian Peng
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  3. Kean Chen
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Correspondence to Yongjin Fang or Yuliang Cao.

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Conflict of interest The authors declare no conflict of interest.

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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Zhao, Y., Peng, J., Chen, K. et al. Boosting the sodium storage performance of Prussian blue analogues via effective etching. Sci. China Chem. 66, 3154–3160 (2023). https://doi.org/10.1007/s11426-023-1824-3

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  • DOI: https://doi.org/10.1007/s11426-023-1824-3

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