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<p>Ordered layered honeycomb structures are crucial for the unique redox mechanism in Co-free Li-rich oxide materials (LMNO). However, oxygen release and irreversible cation migration originating from this distinctive structure during cycling have hindered the further commercialization of LMNO. Herein, we report a strategy to modulate the nanoscale atomic arrangement and electronic band structures by deliberately introducing an integrated short-range disorder in the Li-rich structure with Ce/F dual-doping (denoted as LMNO-CFSD). This work explicitly reveals the induction of this disordered structure and comprehensively investigates its effects on the lattice stability. As a result, the LMNO-CFSD cathode exhibits a high energy density of 934.8 Wh kg<sub>cathode</sub><sup>−1</sup>, and achieves a remarkable lifespan of 800 cycles with 70.1% capacity retention at 1 C in LMNO-CFSD∥ graphite full cells. Spectroscopic studies corroborated by first-principles calculations reveal that this integrated short-range disorder with dual-doping effectively modulates the formation energy of oxygen vacancies. It also tailors the crystal and anionic band structure in the Li-rich phase, fundamentally mitigating detrimental oxygen release and transition metal migration during Li<sup>+</sup> (de)intercalation. Our findings illuminate the crucial role of correlated disorder in enhancing the electrochemical properties of Li-rich layered oxides, thereby offering new design principles for high-performance cathode materials in next-generation lithium batteries.</p>

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Tuning anionic bands and lattice stability by short-range disorder at nanoscale for ultrastable Co-free Li-rich cathode

  • 期刊论文

  • 发表日期：

    2025年2月24日

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  • Ruiqi Zhao,
  • Xingchen Song,
  • Ziheng Zhang,
  • Jinping Zhang,
  • Chenghao Zheng,
  • Jie Zhu,
  • Jie Liu,
  • Kai Zhang,
  • Yanfeng Ma,
  • Chenxi Li,
  • Hongtao Zhang,
  • Yongsheng Chen

摘要

Ordered layered honeycomb structures are crucial for the unique redox mechanism in Co-free Li-rich oxide materials (LMNO). However, oxygen release and irreversible cation migration originating from this distinctive structure during cycling have hindered the further commercialization of LMNO. Herein, we report a strategy to modulate the nanoscale atomic arrangement and electronic band structures by deliberately introducing an integrated short-range disorder in the Li-rich structure with Ce/F dual-doping (denoted as LMNO-CFSD). This work explicitly reveals the induction of this disordered structure and comprehensively investigates its effects on the lattice stability. As a result, the LMNO-CFSD cathode exhibits a high energy density of 934.8 Wh kgcathode−1, and achieves a remarkable lifespan of 800 cycles with 70.1% capacity retention at 1 C in LMNO-CFSD∥ graphite full cells. Spectroscopic studies corroborated by first-principles calculations reveal that this integrated short-range disorder with dual-doping effectively modulates the formation energy of oxygen vacancies. It also tailors the crystal and anionic band structure in the Li-rich phase, fundamentally mitigating detrimental oxygen release and transition metal migration during Li+ (de)intercalation. Our findings illuminate the crucial role of correlated disorder in enhancing the electrochemical properties of Li-rich layered oxides, thereby offering new design principles for high-performance cathode materials in next-generation lithium batteries.