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Mutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxides

Author

Listed:
  • Shaofeng Li

    (SLAC National Accelerator Laboratory
    Dalian University of Technology)

  • Zhisen Jiang

    (SLAC National Accelerator Laboratory)

  • Jiaxiu Han

    (Purdue University)

  • Zhengrui Xu

    (Virginia Tech)

  • Chenxu Wang

    (Stanford University)

  • Hai Huang

    (SLAC National Accelerator Laboratory)

  • Chang Yu

    (Dalian University of Technology)

  • Sang-Jun Lee

    (SLAC National Accelerator Laboratory)

  • Piero Pianetta

    (SLAC National Accelerator Laboratory)

  • Hendrik Ohldag

    (Lawrence Berkeley National Laboratory
    Stanford University
    University of California-Santa Cruz)

  • Jieshan Qiu

    (Dalian University of Technology)

  • Jun-Sik Lee

    (SLAC National Accelerator Laboratory)

  • Feng Lin

    (Virginia Tech)

  • Kejie Zhao

    (Purdue University)

  • Yijin Liu

    (SLAC National Accelerator Laboratory)

Abstract

Surface lattice reconstruction is commonly observed in nickel-rich layered oxide battery cathode materials, causing unsatisfactory high-voltage cycling performance. However, the interplay of the surface chemistry and the bulk microstructure remains largely unexplored due to the intrinsic structural complexity and the lack of integrated diagnostic tools for a thorough investigation at complementary length scales. Herein, by combining nano-resolution X-ray probes in both soft and hard X-ray regimes, we demonstrate correlative surface chemical mapping and bulk microstructure imaging over a single charged LiNi0.8Mn0.1Co0.1O2 (NMC811) secondary particle. We reveal that the sub-particle regions with more micro cracks are associated with more severe surface degradation. A mechanism of mutual modulation between the surface chemistry and the bulk microstructure is formulated based on our experimental observations and finite element modeling. Such a surface-to-bulk reaction coupling effect is fundamentally important for the design of the next generation battery cathode materials.

Suggested Citation

  • Shaofeng Li & Zhisen Jiang & Jiaxiu Han & Zhengrui Xu & Chenxu Wang & Hai Huang & Chang Yu & Sang-Jun Lee & Piero Pianetta & Hendrik Ohldag & Jieshan Qiu & Jun-Sik Lee & Feng Lin & Kejie Zhao & Yijin , 2020. "Mutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxides," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18278-y
    DOI: 10.1038/s41467-020-18278-y
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    Cited by:

    1. Zhongsheng Dai & Zhujie Li & Renjie Chen & Feng Wu & Li Li, 2023. "Defective oxygen inert phase stabilized high-voltage nickel-rich cathode for high-energy lithium-ion batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Zhichen Xue & Nikhil Sharma & Feixiang Wu & Piero Pianetta & Feng Lin & Luxi Li & Kejie Zhao & Yijin Liu, 2023. "Asynchronous domain dynamics and equilibration in layered oxide battery cathode," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    3. Shaofeng Li & Guannan Qian & Xiaomei He & Xiaojing Huang & Sang-Jun Lee & Zhisen Jiang & Yang Yang & Wei-Na Wang & Dechao Meng & Chang Yu & Jun-Sik Lee & Yong S. Chu & Zi-Feng Ma & Piero Pianetta & Ji, 2022. "Thermal-healing of lattice defects for high-energy single-crystalline battery cathodes," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Ziyao Gao & Chenglong Zhao & Kai Zhou & Junru Wu & Yao Tian & Xianming Deng & Lihan Zhang & Kui Lin & Feiyu Kang & Lele Peng & Marnix Wagemaker & Baohua Li, 2024. "Kirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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