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Surface spinel reconstruction to suppress detrimental phase transition for stable LiNi0.8Co0.1Mn0.1O2 cathodes

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Abstract

Nickel-rich layered oxides are attractive cathode for lithium-ion batteries (LIBs) because of the high energy density and low cost. The critical problem is capacity fading caused by the highly reactive metastable phases under voltages of higher than 4.15 V. Herein, we find that facile Ar/H2 plasma treating could produce oxygen vacancies that will readily transform into homogeneous spinel layer (∼ 6 nm) on the LiNi0.8Co0.1Mn0.1O2 (NCM811) surface after a few cycles of lithiation/delithiation procedure. Owing to the structural matching between spinel and layered structure, the diffusion of Li ions could remain fast upon cycling. Besides, the spinel layer is electrochemically inert, which guarantees surface stabilization and inhibits the detrimental phase transition from H2 to H3 at high voltages. Under the protection of the homogeneous spinel layer, the NCM811 electrode shows superior capacity retention of 91.2% after 200 cycles at the current density of 100 mA·g−1. This work proposes a novel strategy of surface reconstruction to stabilize nickel-rich layered oxide materials for LIBs.

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Acknowledgements

This work was financially supported by the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen (No. JCYJ20200109141640095), Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (No. ZDSYS20200421111401738), the Leading Talents of Guangdong Province Program (No. 2016LJ06C536), the Guangdong-Hong Kong-Macao Joint Laboratory (No. 2019B121205001), and the National Natural Science Foundation of China (No. 21875097). Help on scanning electron microscopy (SEM), TEM, inductively coupled plasma-mass spectrometry (ICP-MS), and XRD characterizations from the Core Research Facilities and DFT simulations from the Center for Computational Science and Engineering at Southern University of Science and Technology are gratefully appreciated. The X-ray absorption fine structure (XAFS) experiments were conducted in the BL02U Beamlines at the Shanghai Synchrotron Radiation Facility.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials, Southern University of Science and Technology, Shenzhen, 518055, China

    Qingmeng Gan, Ning Qin, Zhiqiang Li, Shuai Gu, Kemeng Liao, Zhenghe Xu & Zhouguang Lu

  2. Department of Mechanical Engineering, National University of Singapore, Singapore, 117575, Singapore

    Qingmeng Gan & Li Lu

  3. Department of Mechanical Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Hong Kong, 999077, China

    Ning Qin, Shuai Gu & Kaili Zhang

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  1. Qingmeng Gan
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  2. Ning Qin
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  3. Zhiqiang Li
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  5. Kemeng Liao
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  7. Li Lu
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  8. Zhenghe Xu
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  9. Zhouguang Lu
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Correspondence to Zhouguang Lu.

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Gan, Q., Qin, N., Li, Z. et al. Surface spinel reconstruction to suppress detrimental phase transition for stable LiNi0.8Co0.1Mn0.1O2 cathodes. Nano Res. 16, 513–520 (2023). https://doi.org/10.1007/s12274-022-4754-z

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