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Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries

Author

Listed:
  • Feng Lin

    (Lawrence Berkeley National Laboratory)

  • Isaac M. Markus

    (Lawrence Berkeley National Laboratory
    University of California)

  • Dennis Nordlund

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Tsu-Chien Weng

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Mark D. Asta

    (University of California)

  • Huolin L. Xin

    (Center for Functional Nanomaterials, Brookhaven National Laboratory)

  • Marca M. Doeff

    (Lawrence Berkeley National Laboratory)

Abstract

The present study sheds light on the long-standing challenges associated with high-voltage operation of LiNixMnxCo1−2xO2 cathode materials for lithium-ion batteries. Using correlated ensemble-averaged high-throughput X-ray absorption spectroscopy and spatially resolved electron microscopy and spectroscopy, here we report structural reconstruction (formation of a surface reduced layer, to transition) and chemical evolution (formation of a surface reaction layer) at the surface of LiNixMnxCo1−2xO2 particles. These are primarily responsible for the prevailing capacity fading and impedance buildup under high-voltage cycling conditions, as well as the first-cycle coulombic inefficiency. It was found that the surface reconstruction exhibits a strong anisotropic characteristic, which predominantly occurs along lithium diffusion channels. Furthermore, the surface reaction layer is composed of lithium fluoride embedded in a complex organic matrix. This work sets a refined example for the study of surface reconstruction and chemical evolution in battery materials using combined diagnostic tools at complementary length scales.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms4529
    DOI: 10.1038/ncomms4529
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    1. Xinlei Shi & Xiangqian Fan & Yinbo Zhu & Yang Liu & Peiqi Wu & Renhui Jiang & Bao Wu & Heng-An Wu & He Zheng & Jianbo Wang & Xinyi Ji & Yongsheng Chen & Jiajie Liang, 2022. "Pushing detectability and sensitivity for subtle force to new limits with shrinkable nanochannel structured aerogel," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Ermanno Miele & Wesley M. Dose & Ilya Manyakin & Michael H. Frosz & Zachary Ruff & Michael F. L. Volder & Clare P. Grey & Jeremy J. Baumberg & Tijmen G. Euser, 2022. "Hollow-core optical fibre sensors for operando Raman spectroscopy investigation of Li-ion battery liquid electrolytes," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. 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.
    4. Ke Chen & Pallab Barai & Ozgenur Kahvecioglu & Lijun Wu & Krzysztof Z. Pupek & Mingyuan Ge & Lu Ma & Steven N. Ehrlich & Hui Zhong & Yimei Zhu & Venkat Srinivasan & Jianming Bai & Feng Wang, 2024. "Cobalt-free composite-structured cathodes with lithium-stoichiometry control for sustainable lithium-ion batteries," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. 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.
    6. Jeongjin Kim & Youngseok Yu & Tae Won Go & Jean-Jacques Gallet & Fabrice Bournel & Bongjin Simon Mun & Jeong Young Park, 2023. "Revealing CO2 dissociation pathways at vicinal copper (997) interfaces," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    7. Christian M. Julien & Alain Mauger, 2020. "NCA, NCM811, and the Route to Ni-Richer Lithium-Ion Batteries," Energies, MDPI, vol. 13(23), pages 1-46, December.
    8. 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.
    9. Xuelong Wang & Liang Yin & Arthur Ronne & Yiman Zhang & Zilin Hu & Sha Tan & Qinchao Wang & Bohang Song & Mengya Li & Xiaohui Rong & Saul Lapidus & Shize Yang & Enyuan Hu & Jue Liu, 2023. "Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    10. 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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