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Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries

Author

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  • Pengfei Yan

    (Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • Jianming Zheng

    (Energy and Environment Directorate, Pacific Northwest National Laboratory)

  • Meng Gu

    (Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

  • Jie Xiao

    (Energy and Environment Directorate, Pacific Northwest National Laboratory)

  • Ji-Guang Zhang

    (Energy and Environment Directorate, Pacific Northwest National Laboratory)

  • Chong-Min Wang

    (Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory)

Abstract

LiNi1/3Mn1/3Co1/3O2-layered cathode is often fabricated in the form of secondary particles, consisting of densely packed primary particles. This offers advantages for high energy density and alleviation of cathode side reactions/corrosions, but introduces drawbacks such as intergranular cracking. Here, we report unexpected observations on the nucleation and growth of intragranular cracks in a commercial LiNi1/3Mn1/3Co1/3O2 cathode by using advanced scanning transmission electron microscopy. We find the formation of the intragranular cracks is directly associated with high-voltage cycling, an electrochemically driven and diffusion-controlled process. The intragranular cracks are noticed to be characteristically initiated from the grain interior, a consequence of a dislocation-based crack incubation mechanism. This observation is in sharp contrast with general theoretical models, predicting the initiation of intragranular cracks from grain boundaries or particle surfaces. Our study emphasizes that maintaining structural stability is the key step towards high-voltage operation of layered-cathode materials.

Suggested Citation

  • Pengfei Yan & Jianming Zheng & Meng Gu & Jie Xiao & Ji-Guang Zhang & Chong-Min Wang, 2017. "Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14101
    DOI: 10.1038/ncomms14101
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    1. Tongchao Liu & Lei Yu & Jun Lu & Tao Zhou & Xiaojing Huang & Zhonghou Cai & Alvin Dai & Jihyeon Gim & Yang Ren & Xianghui Xiao & Martin V. Holt & Yong S. Chu & Ilke Arslan & Jianguo Wen & Khalil Amine, 2021. "Rational design of mechanically robust Ni-rich cathode materials via concentration gradient strategy," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    2. Danfeng Zhang & Ming Liu & Jiabin Ma & Ke Yang & Zhen Chen & Kaikai Li & Chen Zhang & Yinping Wei & Min Zhou & Peng Wang & Yuanbiao He & Wei Lv & Quan-Hong Yang & Feiyu Kang & Yan-Bing He, 2022. "Lithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Tao Cheng & Zhongtao Ma & Run Gu & Riming Chen & Yingchun Lyu & Anmin Nie & Bingkun Guo, 2018. "Cracks Formation in Lithium-Rich Cathode Materials for Lithium-Ion Batteries during the Electrochemical Process," Energies, MDPI, vol. 11(10), pages 1-10, October.
    4. 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.
    5. Kai Wang & Zhenqi Gu & Zhiwei Xi & Lv Hu & Cheng Ma, 2023. "Li3TiCl6 as ionic conductive and compressible positive electrode active material for all-solid-state lithium-based batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Ho-Young Jang & Donggun Eum & Jiung Cho & Jun Lim & Yeji Lee & Jun-Hyuk Song & Hyeokjun Park & Byunghoon Kim & Do-Hoon Kim & Sung-Pyo Cho & Sugeun Jo & Jae Hoon Heo & Sunyoung Lee & Jongwoo Lim & Kisu, 2024. "Structurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    7. Junbo Zhang & Haikuo Zhang & Suting Weng & Ruhong Li & Di Lu & Tao Deng & Shuoqing Zhang & Ling Lv & Jiacheng Qi & Xuezhang Xiao & Liwu Fan & Shujiang Geng & Fuhui Wang & Lixin Chen & Malachi Noked & , 2023. "Multifunctional solvent molecule design enables high-voltage Li-ion batteries," Nature Communications, Nature, vol. 14(1), pages 1-14, December.

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