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<p>The vehicle industry’s increasing demand for electrification necessitates the removal of expensive and rare cobalt from current high-energy batteries. However, eliminating cobalt poses challenges due to its vital role in maintaining the layered structural ordering and cycling stability of commonly used Li(NiMnCo)O<sub>2</sub> cathodes. As an alternative to conventional layered oxide designs, we report a lithium nickelate cathode with a composite structure comprising major stoichiometric layered and minor rocksalt phases within the same oxygen lattice. This material outperforms conventional designs by maintaining stable battery operation at voltages up to 4.8 V vs. Li|Li<sup>+</sup>, with 88% capacity retention after 1000 cycles at 2C. The topotaxial-growth-enabled interlock between the two components mitigates chemo-mechanical degradation, offering a promising pathway to cobalt-free cathodes. Additionally, we reveal a miscibility gap in the Li-Ni-O system that enables kinetic adjustment of composition and structure during sintering, thereby tuning the functionality of high-energy cathodes.</p>

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Topotaxially grown composite cathodes for cobalt-free high-energy long-life Li-ion batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月20日

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  • Junyi Yao,
  • Sizhan Liu,
  • Wujun Zhang,
  • Lijun Wu,
  • Zhenjie Zhang,
  • Ping He,
  • Yanbin Shen,
  • Liwei Chen,
  • Mingyuan Ge,
  • Lu Ma,
  • Xiaotian Zhu,
  • Kaihua Xu,
  • Kun Zhang,
  • Feng Wang,
  • Jianqing Zhao,
  • Jianming Bai

摘要

The vehicle industry’s increasing demand for electrification necessitates the removal of expensive and rare cobalt from current high-energy batteries. However, eliminating cobalt poses challenges due to its vital role in maintaining the layered structural ordering and cycling stability of commonly used Li(NiMnCo)O2 cathodes. As an alternative to conventional layered oxide designs, we report a lithium nickelate cathode with a composite structure comprising major stoichiometric layered and minor rocksalt phases within the same oxygen lattice. This material outperforms conventional designs by maintaining stable battery operation at voltages up to 4.8 V vs. Li|Li+, with 88% capacity retention after 1000 cycles at 2C. The topotaxial-growth-enabled interlock between the two components mitigates chemo-mechanical degradation, offering a promising pathway to cobalt-free cathodes. Additionally, we reveal a miscibility gap in the Li-Ni-O system that enables kinetic adjustment of composition and structure during sintering, thereby tuning the functionality of high-energy cathodes.