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<p>Structure evolution and surface reactivity have long been regarded as the most crucial points for studying Ni-rich positive electrodes for Li-ion batteries. Unfortunately, the influence of Li occupancy as a single factor on electro-chemomechanical stability has been overlooked and is missing, owing to the challenge of Li determination in the lattice. Here, a comprehensive analysis reveals different Li occupancies and related structural domains (Ni/Li exchange, Li<sub><i>a</i></sub>XO<sub><i>b</i></sub>, Li/Mn/X(Ni) ordering domains, X = Nb<sup>5+</sup>, W<sup>6+</sup>, and Mo<sup>6+</sup>) by using a combination of Li-sensitive characterization techniques. By introducing a Li-regulation strategy, the relative ratio of each domain is effectively tuned in the Ni-rich positive electrodes. Through tuning, two specific positive electrodes are designed, exhibiting notable improvement in battery cyclability. The specific Li structural units induce significant changes in redox mechanisms. This Li-occupancy-tuning approach highlights the necessity of focusing on Li distribution and opens up ideas for designing advanced Ni-rich positive electrodes with high durability.</p>

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Tuning Li occupancy and local structures for advanced Co-free Ni-rich positive electrodes

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年3月5日

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  • Hang Li,
  • Hao Liu,
  • Shunrui Luo,
  • Jordi Arbiol,
  • Emmanuelle Suard,
  • Thomas Bergfeldt,
  • Alexander Missyul,
  • Volodymyr Baran,
  • Stefan Mangold,
  • Yongchao Zhang,
  • Weibo Hua,
  • Michael Knapp,
  • Helmut Ehrenberg,
  • Feng Pan,
  • Sylvio Indris

摘要

Structure evolution and surface reactivity have long been regarded as the most crucial points for studying Ni-rich positive electrodes for Li-ion batteries. Unfortunately, the influence of Li occupancy as a single factor on electro-chemomechanical stability has been overlooked and is missing, owing to the challenge of Li determination in the lattice. Here, a comprehensive analysis reveals different Li occupancies and related structural domains (Ni/Li exchange, LiaXOb, Li/Mn/X(Ni) ordering domains, X = Nb5+, W6+, and Mo6+) by using a combination of Li-sensitive characterization techniques. By introducing a Li-regulation strategy, the relative ratio of each domain is effectively tuned in the Ni-rich positive electrodes. Through tuning, two specific positive electrodes are designed, exhibiting notable improvement in battery cyclability. The specific Li structural units induce significant changes in redox mechanisms. This Li-occupancy-tuning approach highlights the necessity of focusing on Li distribution and opens up ideas for designing advanced Ni-rich positive electrodes with high durability.