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<p>LiCoO₂ (LCO) cathodes suffer from severe interfacial degradation, including cobalt dissolution, oxygen loss, and structural collapse, when cycled at high voltages (&gt; 4.6&#xa0;V), which limits their practical application. To address this issue, we propose a heterojunction engineering strategy via surface coating with lithium zirconium phosphate (Li₂Zr(PO₄)₂, LZP). The optimized LCO@LZP cathode delivers an ultrahigh initial discharge capacity of 178.1 mAh·g<sup>− 1</sup> at 1&#xa0;C (3.0–4.6&#xa0;V) and retains 86.3% of its capacity after 200 cycles, significantly outperforming bare LCO (76.0%). It also exhibits enhanced rate capability (108.7 mAh·g<sup>− 1</sup> at 10&#xa0;C) and near-complete capacity recovery (99.7%) upon returning to 0.1&#xa0;C. Mechanistic studies reveal that the LZP coating stabilizes lattice oxygen through robust Zr–O and P–O bonds, suppresses electrolyte decomposition to form a thin and inorganic-rich cathode electrolyte interphase (CEI), and enhances Li<sup>+</sup> diffusion kinetics (DLi<sup>+</sup> = 8.51 × 10<sup>− 12</sup> cm<sup>2</sup>·s<sup>− 1</sup>, 2.4 times higher than bare LCO). DFT calculations further confirm that the LCO/LZP heterojunction reduces oxygen charge compensation and creates an internal electric field that facilitates ion transport while inhibiting electron leakage. This work provides a scalable surface-modification strategy for developing high-energy-density LCO cathodes for next-generation lithium-ion batteries.</p>

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Cation-anion synergistic stabilization at the heterointerface for ultra-stable 4.6 V LiCoO2 cathodes

  • 期刊论文

  • 发表日期：

    2026年3月17日

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  • Keying Wu,
  • Haiwen Tang,
  • Yao Liu,
  • Dan Wang,
  • Jinjin Jiang,
  • Liusi Yu,
  • Sujun Wang,
  • Lei Chen,
  • Kai Tang

摘要

LiCoO₂ (LCO) cathodes suffer from severe interfacial degradation, including cobalt dissolution, oxygen loss, and structural collapse, when cycled at high voltages (> 4.6 V), which limits their practical application. To address this issue, we propose a heterojunction engineering strategy via surface coating with lithium zirconium phosphate (Li₂Zr(PO₄)₂, LZP). The optimized LCO@LZP cathode delivers an ultrahigh initial discharge capacity of 178.1 mAh·g− 1 at 1 C (3.0–4.6 V) and retains 86.3% of its capacity after 200 cycles, significantly outperforming bare LCO (76.0%). It also exhibits enhanced rate capability (108.7 mAh·g− 1 at 10 C) and near-complete capacity recovery (99.7%) upon returning to 0.1 C. Mechanistic studies reveal that the LZP coating stabilizes lattice oxygen through robust Zr–O and P–O bonds, suppresses electrolyte decomposition to form a thin and inorganic-rich cathode electrolyte interphase (CEI), and enhances Li+ diffusion kinetics (DLi+ = 8.51 × 10− 12 cm2·s− 1, 2.4 times higher than bare LCO). DFT calculations further confirm that the LCO/LZP heterojunction reduces oxygen charge compensation and creates an internal electric field that facilitates ion transport while inhibiting electron leakage. This work provides a scalable surface-modification strategy for developing high-energy-density LCO cathodes for next-generation lithium-ion batteries.