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Realizing High Capacity and Zero Strain in Layered Oxide Cathodes via Lithium Dual-Site Substitution for Sodium-Ion Batteries

  • Zhonghan Wu
    Zhonghan Wu
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
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  • Youxuan Ni
    Youxuan Ni
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    More by Youxuan Ni
  • Sha Tan
    Sha Tan
    Chemistry Division, Brookhaven National Laboratory Upton, New York 11973, United States
    More by Sha Tan
  • Enyuan Hu
    Enyuan Hu
    Chemistry Division, Brookhaven National Laboratory Upton, New York 11973, United States
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  • Lunhua He
    Lunhua He
    Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, P. R. China
    Songshan Lake Materials Laboratory, Dongguan 523808, P. R. China
    Spallation Neutron Source Science Center, Dongguan 523803, P. R. China
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  • Jiuding Liu
    Jiuding Liu
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    More by Jiuding Liu
  • Machuan Hou
    Machuan Hou
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    More by Machuan Hou
  • Peixin Jiao
    Peixin Jiao
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    More by Peixin Jiao
  • Kai Zhang*
    Kai Zhang
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, P. R. China
    *Email: [email protected]
    More by Kai Zhang
  • Fangyi Cheng*
    Fangyi Cheng
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, P. R. China
    *Email: [email protected]
    More by Fangyi Cheng
  • , and 
  • Jun Chen
    Jun Chen
    Frontiers Science Center for New Organic Matter, Renewable Energy Conversion and Storage Center (RECAST), Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, P. R. China
    Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, P. R. China
    More by Jun Chen
Cite this: J. Am. Chem. Soc. 2023, 145, 17, 9596–9606
Publication Date (Web):April 14, 2023
https://doi.org/10.1021/jacs.3c00117
Copyright © 2023 American Chemical Society

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    Abstract

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    Sodium-ion batteries have garnered unprecedented attention as an electrochemical energy storage technology, but it remains challenging to design high-energy-density cathode materials with low structural strain during the dynamic (de)sodiation processes. Herein, we report a P2-layered lithium dual-site-substituted Na0.7Li0.03[Mg0.15Li0.07Mn0.75]O2 (NMLMO) cathode material, in which Li ions occupy both transition-metal (TM) and alkali-metal (AM) sites. The combination of theoretical calculations and experimental characterizations reveals that LiTM creates Na–O–Li electronic configurations to boost the capacity derived from the oxygen anionic redox, while LiAM serves as LiO6 prismatic pillars to stabilize the layered structure through suppressing the detrimental phase transitions. As a result, NMLMO delivers a high specific capacity of 266 mAh g–1 and simultaneously exhibits the nearly zero-strain characteristic within a wide voltage range of 1.5–4.6 V. Our findings highlight the effective way of dual-site substitution to break the capacity–stability trade-off in cathode materials for advanced rechargeable batteries.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c00117.

    • Details of material synthesis and characterizations, electrochemical measurements, and theoretical calculations; NMR, XPS, XAS, SEM, TEM, XRD, NPD, EDS, ICP and DEMS data of NMMO and NMLMO; electrochemical results; crystallographic parameters of NMMO and NMLMO; lattice parameters of NMMO and NMLMO; and fitted EXAFS parameters of NMMO and NMLMO (PDF)

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    Cited By

    This article is cited by 6 publications.

    1. Yameng Fan, Emilia Olsson, Bernt Johannessen, Anita M. D’Angelo, Lars Thomsen, Bruce Cowie, Lachlan Smillie, Gemeng Liang, Yaojie Lei, Guyue Bo, Yunlong Zhao, Wei Kong Pang, Qiong Cai, Zaiping Guo. Manipulation of Transition Metal Migration via Cr-Doping for Better-Performance Li-Rich, Co-Free Cathodes. ACS Energy Letters 2024, 9 (2) , 487-496. https://doi.org/10.1021/acsenergylett.3c02509
    2. Zeren Chen, Runxian Jiao, Hang Liu, Hualu Wang, Xiangyu Liu, Xiaoyu Zhang, Min Jia, Yuanping Chen, Xiaohong Yan. Coupling the Electronic Distribution and Oxygen Redox Potential via Cu Substitution of Layered Oxide Cathodes for Sodium-Ion Batteries. ACS Sustainable Chemistry & Engineering 2024, 12 (2) , 816-825. https://doi.org/10.1021/acssuschemeng.3c05369
    3. Youmei Chen, Sheng Feng, Jiayu Chen, Yan Lu, Meifen Wu, Xiangwei Wu, Zhaoyin Wen. Pulse-Assisted Low-Temperature Sintering to Enhance the Fast-Charging Capability for P2-Layered Na-Based Cathodes. ACS Applied Energy Materials 2023, 6 (24) , 12421-12431. https://doi.org/10.1021/acsaem.3c02290
    4. Yao Wang, Xudong Zhao, Junteng Jin, Qiuyu Shen, Yang Hu, Xiaobai Song, Han Li, Xuanhui Qu, Lifang Jiao, Yongchang Liu. Boosting the Reversibility and Kinetics of Anionic Redox Chemistry in Sodium-Ion Oxide Cathodes via Reductive Coupling Mechanism. Journal of the American Chemical Society 2023, 145 (41) , 22708-22719. https://doi.org/10.1021/jacs.3c08070
    5. Xiaoxia Yang, Suning Wang, Hang Li, Jiali Peng, Wen-Jing Zeng, Hsin-Jung Tsai, Sung-Fu Hung, Sylvio Indris, Fujun Li, Weibo Hua. Boosting the Ultrastable High-Na-Content P2-type Layered Cathode Materials with Zero-Strain Cation Storage via a Lithium Dual-Site Substitution Approach. ACS Nano 2023, 17 (18) , 18616-18628. https://doi.org/10.1021/acsnano.3c07625
    6. Kai Fang, Yonglin Tang, Junjie Liu, Zhefei Sun, Xiaotong Wang, Leiyu Chen, Xiaohong Wu, Qiaobao Zhang, Li Zhang, Yu Qiao, Shi-Gang Sun. Injecting Excess Na into a P2-Type Layered Oxide Cathode to Achieve Presodiation in a Na-Ion Full Cell. Nano Letters 2023, 23 (14) , 6681-6688. https://doi.org/10.1021/acs.nanolett.3c01890

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