<p>Nickel-rich 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) cathodes, pivotal for high-energy–density lithium-ion batteries, face severe challenges from surface residual lithium compounds and hydrofluoric acid (HF)-induced degradation. These issues accelerate capacity fading, exacerbate interfacial polarization, and compromise safety. To address these issues, we proposed a scalable CeF<sub>3</sub>/H<sub>3</sub>BO<sub>3</sub> hybrid coating strategy for LiNi<sub>0.82</sub>Co<sub>0.12</sub>Mn<sub>0.06</sub>O<sub>2</sub> cathodes. The CeF<sub>3</sub> nanoparticles served as a robust physical barrier, effectively scavenging HF, while the LiBO<sub>2</sub> layer derived from H<sub>3</sub>BO<sub>3</sub> eliminated residual Li<sub>2</sub>CO<sub>3</sub> through chemical conversion and established rapid Li<sup>+</sup> transport pathways. Dynamic B-O bond reorganization enabled self-repair of coating defects, synergistically suppressing interfacial polarization and maintaining structural integrity. Electrochemical evaluations demonstrated that the hybrid-coated cathode achieves 94% capacity retention after 200 cycles at 1C (2.8–4.3&#xa0;V), significantly outperforming the pristine NCM (56.3%). Additionally, the modified cathode exhibits enhanced air stability, with suppressed H<sub>2</sub>O/CO<sub>2</sub> infiltration, and delivers 80% capacity retention after 1000 cycles in practical pouch cells. This work provides a cost-effective and industrially viable solution to simultaneously mitigate HF corrosion, residual lithium accumulation, and cathode–electrolyte interphase instability, paving the way for durable high-energy–density batteries.</p> Graphical abstract <p></p>

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Synergistic LiBO2/CeF3 hybrid coating engineering for chemically stabilized cathode–electrolyte interphase in nickel-rich cathodes

  • Xin-Kang Li,
  • Li-Jun Xiong,
  • Bai-Yao Gan,
  • Hao-Tian Gong,
  • Yin Ma,
  • Li-Xiong Bai,
  • Jian Zhu,
  • Chun-Xian Zhou,
  • Jiang Yin,
  • Xiang-Ping Chen,
  • Li-Shan Yang

摘要

Nickel-rich LiNixCoyMn1−xyO2 (NCM) cathodes, pivotal for high-energy–density lithium-ion batteries, face severe challenges from surface residual lithium compounds and hydrofluoric acid (HF)-induced degradation. These issues accelerate capacity fading, exacerbate interfacial polarization, and compromise safety. To address these issues, we proposed a scalable CeF3/H3BO3 hybrid coating strategy for LiNi0.82Co0.12Mn0.06O2 cathodes. The CeF3 nanoparticles served as a robust physical barrier, effectively scavenging HF, while the LiBO2 layer derived from H3BO3 eliminated residual Li2CO3 through chemical conversion and established rapid Li+ transport pathways. Dynamic B-O bond reorganization enabled self-repair of coating defects, synergistically suppressing interfacial polarization and maintaining structural integrity. Electrochemical evaluations demonstrated that the hybrid-coated cathode achieves 94% capacity retention after 200 cycles at 1C (2.8–4.3 V), significantly outperforming the pristine NCM (56.3%). Additionally, the modified cathode exhibits enhanced air stability, with suppressed H2O/CO2 infiltration, and delivers 80% capacity retention after 1000 cycles in practical pouch cells. This work provides a cost-effective and industrially viable solution to simultaneously mitigate HF corrosion, residual lithium accumulation, and cathode–electrolyte interphase instability, paving the way for durable high-energy–density batteries.

Graphical abstract