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<p>Single-crystalline layered oxides offer a promising solution to mitigate the rapid capacity decay observed in conventional polycrystalline nickel-rich oxide cathodes. However, achieving both morphological (large grain size) and structural (cation-disorder-free) control in single crystals remains challenging due to the trade-off between grain growth and phase stability, particularly at high-nickel contents. Here we report cation-disorder-free ultrahigh-nickel single-crystalline oxide cathodes with ~10-μm particle sizes, comparable to commercial secondary particles, that deliver high volumetric capacity and stable cycling. These single crystals withstand calendering and resist intra-granular cracking, achieving electrode densities of up to 77% of the theoretical crystal density. The improved stability is linked to reduced structural strain and modified glide behaviour due to the absence of cation disorder, emphasizing its critical role in chemomechanical behaviour. Additionally, gas evolution is reduced by a factor of 25, and the thermal onset temperature drops by more than 20 °C at ~4.5 V versus Li/Li<sup>+</sup>, underscoring superior safety features and energy density potential.</p>

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Approaching the theoretical density limit of ultrahigh-nickel cathodes via cation-disorder-free 10-μm single-crystalline particles

  • 期刊论文

  • 发表日期：

    2026年1月2日

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  • Youngjun Jeon,
  • Donggun Eum,
  • Ho-Young Jang,
  • Young-Uk Park,
  • Mincheol Beak,
  • Kyoungoh Kim,
  • Dae Soo Jung,
  • Minsik Oh,
  • In-Suk Choi,
  • Kun-Hee Ko,
  • Youngsin Kim,
  • Jihyeon Kim,
  • Sangwook Han,
  • Kisuk Kang

摘要

Single-crystalline layered oxides offer a promising solution to mitigate the rapid capacity decay observed in conventional polycrystalline nickel-rich oxide cathodes. However, achieving both morphological (large grain size) and structural (cation-disorder-free) control in single crystals remains challenging due to the trade-off between grain growth and phase stability, particularly at high-nickel contents. Here we report cation-disorder-free ultrahigh-nickel single-crystalline oxide cathodes with ~10-μm particle sizes, comparable to commercial secondary particles, that deliver high volumetric capacity and stable cycling. These single crystals withstand calendering and resist intra-granular cracking, achieving electrode densities of up to 77% of the theoretical crystal density. The improved stability is linked to reduced structural strain and modified glide behaviour due to the absence of cation disorder, emphasizing its critical role in chemomechanical behaviour. Additionally, gas evolution is reduced by a factor of 25, and the thermal onset temperature drops by more than 20 °C at ~4.5 V versus Li/Li+, underscoring superior safety features and energy density potential.