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<p>To improve the cycling stability of nickel-rich single-crystal LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub> under high operating voltage while avoiding the impact on the main structure caused by conventional secondary calcination modification methods, a rock-salt phase interface layer (&lt; 10&#xa0;nm) is constructed on the surface of LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub> through low-temperature epitaxial self-growth without introducing heterogeneous atoms. In situ X-ray diffraction (XRD) analysis reveals the formation of a metastable transition phase during the deep delithiation process. Notably, the presence of the rock-salt phase layer remarkably suppresses the persistence of the metastable transition phase. Further investigation using differential capacitance curve (d<i>Q</i>/d<i>V</i>) demonstrates that suppressing this metastable phase improves the reversibility of the H2–H3 phase transition, thus facilitating long-term cycling stability of the modified sample at 4.5&#xa0;V. This work presents a novel and effective interface reconstruction approach for the modification of single-crystal nickel-rich cathodes.</p> Graphical Abstract <p></p>

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Enhanced cycling stability of nickel-rich single-crystal LiNi0.83Co0.12Mn0.05O2 at high voltage via low-temperature epitaxial rock-salt interface engineering

  • 期刊论文

  • 发表日期：

    2025年9月12日

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  • Qinglu Fan,
  • Xia Li,
  • Yankui Cheng,
  • Yanjie Hu,
  • Wencheng Ma,
  • Zehua Chen

摘要

To improve the cycling stability of nickel-rich single-crystal LiNi0.83Co0.12Mn0.05O2 under high operating voltage while avoiding the impact on the main structure caused by conventional secondary calcination modification methods, a rock-salt phase interface layer (< 10 nm) is constructed on the surface of LiNi0.83Co0.12Mn0.05O2 through low-temperature epitaxial self-growth without introducing heterogeneous atoms. In situ X-ray diffraction (XRD) analysis reveals the formation of a metastable transition phase during the deep delithiation process. Notably, the presence of the rock-salt phase layer remarkably suppresses the persistence of the metastable transition phase. Further investigation using differential capacitance curve (dQ/dV) demonstrates that suppressing this metastable phase improves the reversibility of the H2–H3 phase transition, thus facilitating long-term cycling stability of the modified sample at 4.5 V. This work presents a novel and effective interface reconstruction approach for the modification of single-crystal nickel-rich cathodes.

Graphical Abstract