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Realizing High Capacity and Zero Strain in Layered Oxide Cathodes via Lithium Dual-Site Substitution for Sodium-Ion Batteries
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    Realizing High Capacity and Zero Strain in Layered Oxide Cathodes via Lithium Dual-Site Substitution for Sodium-Ion Batteries
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    • 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
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    • 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
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    • 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]
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    • 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]
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    • 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
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2023, 145, 17, 9596–9606
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c00117
    Published April 14, 2023
    Copyright © 2023 American Chemical Society

    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.

    Copyright © 2023 American Chemical Society

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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/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

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    This article is cited by 11 publications.

    1. Yang Yu, Qianjiang Mao, Deniz Wong, Rui Gao, Lirong Zheng, Wenyun Yang, Jinbo Yang, Nian Zhang, Zeyu Li, Christian Schulz, Xiangfeng Liu. Ribbon-Ordered Superlattice Enables Reversible Anion Redox and Stable High-Voltage Na-Ion Battery Cathodes. Journal of the American Chemical Society 2024, 146 (32) , 22220-22235. https://doi.org/10.1021/jacs.4c02782
    2. Haojie Dong, Haoliang Liu, Yu-Jie Guo, Yi-Hu Feng, Xu Zhu, Shao-Wen Xu, Fengxiang Sui, Lianzheng Yu, Mengting Liu, Jin-Zhi Guo, Ya-Xia Yin, Bing Xiao, Xing-Long Wu, Yu-Guo Guo, Peng-Fei Wang. Lithium Orbital Hybridization Chemistry to Stimulate Oxygen Redox with Reversible Phase Evolution in Sodium-Layered Oxide Cathodes. Journal of the American Chemical Society 2024, 146 (32) , 22335-22347. https://doi.org/10.1021/jacs.4c04814
    3. Jiayuan Zhang, Xiang Li. Perspective on Phase Transition in Layered Oxide Cathodes for Sodium-Ion Batteries: Mechanism, Influenced Factors, and Inhibition Strategies. Energy & Fuels 2024, 38 (15) , 13906-13933. https://doi.org/10.1021/acs.energyfuels.4c02631
    4. Yujin Zhou, Lanyan Li, Haisheng Lin, Zhongyun Ma, Xianyou Wang, Guozhao Fang, Zhigao Luo. Reversible Oxygen Redox Chemistry in High-Entropy P2-Type Manganese-Based Cathodes via Self-Regulating Mechanism. ACS Applied Materials & Interfaces 2024, 16 (26) , 33539-33547. https://doi.org/10.1021/acsami.4c05876
    5. Sidra Jamil, Farhan Mudasar, Tiange Yuan, Muhammad Fasehullah, Ghulam Ali, Keun Hwa Chae, Oleksandr Voznyy, Yiqiang Zhan, Maowen Xu. Sb-Doped Biphasic P2/O3-Type Mn-Rich Layered Oxide Cathode Material for High-Performance Sodium-Ion Batteries. ACS Applied Materials & Interfaces 2024, 16 (12) , 14669-14679. https://doi.org/10.1021/acsami.3c15667
    6. 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
    7. 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
    8. 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
    9. 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
    10. 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
    11. 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

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2023, 145, 17, 9596–9606
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c00117
    Published April 14, 2023
    Copyright © 2023 American Chemical Society

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