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Thermal processing to modulate surface chemistry and bulk charge distribution in nickel-rich layered lithium positive electrodes

Author

Listed:
  • Huabin Sun

    (Virginia Tech)

  • Zhijie Yang

    (Virginia Tech)

  • Rupayan Ghosh

    (Virginia Tech)

  • Sooyeon Hwang

    (Brookhaven National Laboratory)

  • Anyang Hu

    (Virginia Tech)

  • Yuxin Zhang

    (Virginia Tech)

  • Jue Liu

    (Oak Ridge National Laboratory)

  • Chengjun Sun

    (Argonne National Laboratory)

  • Sami Sainio

    (SLAC National Accelerator Laboratory)

  • Dennis Nordlund

    (SLAC National Accelerator Laboratory)

  • Xianghui Xiao

    (Brookhaven National Laboratory)

  • Feng Lin

    (Virginia Tech
    Virginia Tech)

Abstract

The broader application of nickel-rich layered oxides as positive electrode materials for lithium-ion batteries has been hindered by their high manufacturing cost and inferior cycling stability. Thermal processing, which is integral to electrode materials manufacturing and fundamental in materials science, has not been fully utilized to design advanced positive electrode materials. Herein, we demonstrate the capability of using quenching heat treatment to regulate Li distribution and modulate electronic structure near particle surface. The resulting materials exhibit less parasitic reactions with the electrolyte and an improved charge distribution homogeneity in secondary particles, leading to more stable cycling performance at high voltages (4.5 V vs Li/Li+). Our synchrotron X-ray analyses reveal the underlying interplay between surface structure and bulk charge distribution in positive electrode materials particles. While strategies used to stabilize positive electrode materials through compositional control, surface modification, and electrolyte engineering have become mature, thermal processing can be advantageous to further improve positive electrode materials manufacturing.

Suggested Citation

  • Huabin Sun & Zhijie Yang & Rupayan Ghosh & Sooyeon Hwang & Anyang Hu & Yuxin Zhang & Jue Liu & Chengjun Sun & Sami Sainio & Dennis Nordlund & Xianghui Xiao & Feng Lin, 2025. "Thermal processing to modulate surface chemistry and bulk charge distribution in nickel-rich layered lithium positive electrodes," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56075-7
    DOI: 10.1038/s41467-025-56075-7
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    References listed on IDEAS

    as
    1. Feng Lin & Isaac M. Markus & Dennis Nordlund & Tsu-Chien Weng & Mark D. Asta & Huolin L. Xin & Marca M. Doeff, 2014. "Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries," Nature Communications, Nature, vol. 5(1), pages 1-9, May.
    2. Xing Ou & Tongchao Liu & Wentao Zhong & Xinming Fan & Xueyi Guo & Xiaojing Huang & Liang Cao & Junhua Hu & Bao Zhang & Yong S. Chu & Guorong Hu & Zhang Lin & Mouad Dahbi & Jones Alami & Khalil Amine &, 2022. "Enabling high energy lithium metal batteries via single-crystal Ni-rich cathode material co-doping strategy," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Zhengrui Xu & Zhisen Jiang & Chunguang Kuai & Rong Xu & Changdong Qin & Yan Zhang & Muhammad Mominur Rahman & Chenxi Wei & Dennis Nordlund & Cheng-Jun Sun & Xianghui Xiao & Xi-Wen Du & Kejie Zhao & Pe, 2020. "Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    4. 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.
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