<p>The Ni-rich layered cathode materials LiNi<sub><i>x</i></sub>Co<sub><i>y</i></sub>Mn<sub>1−<i>x</i>−<i>y</i></sub>O<sub>2</sub> (NCM), which have a high energy density, are crucial in the strategic formulation of next-generation high-performance lithium-ion batteries (LIBs), particularly for cathode materials with Ni ⩾ 0.9. Although advances in NCM cathodes have made them competitive in terms of capacity and cost, persistent challenges such as surface chemical instability (electrolyte-driven surface degradation) and poor mechanical integrity (lattice oxygen evolution and anisotropic microcracking) of the cathodes remain. Addressing these limitations requires coordinated strategies spanning from atomic-level dopant engineering to macroscopic electrode architectural innovations to enable viable large-scale deployment. Extensive research has been conducted on the structural instability caused by an increase in the Ni content, but a comprehensive understanding of its underlying mechanisms and effective modification strategies for next-generation nickel-rich cathodes is lacking. Hence, we provide a thorough overview of the latest findings on microstructural degradation mechanisms in Ni-rich cathodes, delve into recent effective modification strategies and cutting-edge characterization methods, and finally, examine future research directions and limitations. This review elucidates the challenges facing ultrahigh-nickel cathodes and offers new insights into promising research avenues.</p> Graphical Abstract <p></p>

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Exploring Degradation Mechanisms and Recent Developments in High-Nickel Layered Cathodes for Lithium Batteries

  • Guiquan Zhao,
  • Yongjiang Sun,
  • Hang Ma,
  • Futong Ren,
  • Wenjin Huang,
  • Pujia Cheng,
  • Genfu Zhao,
  • Qing Liu,
  • Qi An,
  • Li Yang,
  • Lingyan Duan,
  • Mengjiao Sun,
  • Kun Zeng,
  • Xin Wang,
  • Hong Guo

摘要

The Ni-rich layered cathode materials LiNixCoyMn1−xyO2 (NCM), which have a high energy density, are crucial in the strategic formulation of next-generation high-performance lithium-ion batteries (LIBs), particularly for cathode materials with Ni ⩾ 0.9. Although advances in NCM cathodes have made them competitive in terms of capacity and cost, persistent challenges such as surface chemical instability (electrolyte-driven surface degradation) and poor mechanical integrity (lattice oxygen evolution and anisotropic microcracking) of the cathodes remain. Addressing these limitations requires coordinated strategies spanning from atomic-level dopant engineering to macroscopic electrode architectural innovations to enable viable large-scale deployment. Extensive research has been conducted on the structural instability caused by an increase in the Ni content, but a comprehensive understanding of its underlying mechanisms and effective modification strategies for next-generation nickel-rich cathodes is lacking. Hence, we provide a thorough overview of the latest findings on microstructural degradation mechanisms in Ni-rich cathodes, delve into recent effective modification strategies and cutting-edge characterization methods, and finally, examine future research directions and limitations. This review elucidates the challenges facing ultrahigh-nickel cathodes and offers new insights into promising research avenues.

Graphical Abstract