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Exploring the Charge Compensation Mechanism of P2-Type Na 0.6 Mg 0.3 Mn 0.7 O 2 Cathode Materials for Advanced Sodium-Ion Batteries

Author

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  • Chen Cheng

    (Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 199 Ren’ai Road, Suzhou 215123, China)

  • Manling Ding

    (Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 199 Ren’ai Road, Suzhou 215123, China)

  • Tianran Yan

    (Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 199 Ren’ai Road, Suzhou 215123, China)

  • Kehua Dai

    (College of Chemistry, Tianjin Normal University, Tianjin 300387, China)

  • Jing Mao

    (School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China)

  • Nian Zhang

    (State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China)

  • Liang Zhang

    (Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 199 Ren’ai Road, Suzhou 215123, China)

  • Jinghua Guo

    (Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA
    Department of Chemistry and Biochemistry, University of California, Santa Cruz, CA 95064, USA)

Abstract

P2-type sodium layered transition metal oxides have been intensively investigated as promising cathode materials for sodium-ion batteries (SIBs) by virtue of their high specific capacity and high operating voltage. However, they suffer from problems of voltage decay, capacity fading, and structural deterioration, which hinder their practical application. Therefore, a mechanistic understanding of the cationic/anionic redox activity and capacity fading is indispensable for the further improvement of electrochemical performance. Here, a prototype cathode material of P2-type Na 0.6 Mg 0.3 Mn 0.7 O 2 is comprehensively investigated, which presents both cationic and anionic redox behaviors during the cycling process. By a combination of soft X-ray absorption spectroscopy and electroanalytical methods, we unambiguously reveal that only oxygen redox reaction is involved in the initial charge process, then both oxygen and manganese participate in the charge compensation in the following discharge process. In addition, a gradient distribution of Mn valence state from surface to bulk is disclosed, which could be mainly related to the irreversible oxygen activity during the charge process. Furthermore, we find that the average oxidation state of Mn is reduced upon extended cycles, leading to the noticeable capacity fading. Our results provide deeper insights into the intrinsic cationic/anionic redox mechanism of P2-type materials, which is vital for the rational design and optimization of advanced cathode materials for SIBs.

Suggested Citation

  • Chen Cheng & Manling Ding & Tianran Yan & Kehua Dai & Jing Mao & Nian Zhang & Liang Zhang & Jinghua Guo, 2020. "Exploring the Charge Compensation Mechanism of P2-Type Na 0.6 Mg 0.3 Mn 0.7 O 2 Cathode Materials for Advanced Sodium-Ion Batteries," Energies, MDPI, vol. 13(21), pages 1-12, November.
    • Handle: RePEc:gam:jeners:v:13:y:2020:i:21:p:5729-:d:438859
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    References listed on IDEAS

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    1. Benoit Mortemard de Boisse & Guandong Liu & Jiangtao Ma & Shin-ichi Nishimura & Sai-Cheong Chung & Hisao Kiuchi & Yoshihisa Harada & Jun Kikkawa & Yoshio Kobayashi & Masashi Okubo & Atsuo Yamada, 2016. "Intermediate honeycomb ordering to trigger oxygen redox chemistry in layered battery electrode," Nature Communications, Nature, vol. 7(1), pages 1-9, June.
    2. Qianqian Li & Zhenpeng Yao & Eungje Lee & Yaobin Xu & Michael M. Thackeray & Chris Wolverton & Vinayak P. Dravid & Jinsong Wu, 2019. "Dynamic imaging of crystalline defects in lithium-manganese oxide electrodes during electrochemical activation to high voltage," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
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