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<p>The ever-increasing demand for lithium-ion batteries has necessitated the development of high-performance cathode materials. However, previous studies have predominantly focused on crystal cathodes comprising the octahedral coordination of metal atoms and a well-ordered layered topology. This omits other cathode materials with other structures or coordination that could potentially surpass conventional counterparts in terms of performance. Here, using X-ray diffraction, resonant inelastic X-ray scattering and X-ray absorption near-edge spectra experiments, we investigated an amorphous Li–V–O–F cathode (a-LVOF) with tetrahedral coordination and elucidated an O–O formal redox mechanism at a moderate voltage of 4.1 V, without a conventional octahedral Li–O–Li configuration. The electrochemically amorphized material fosters randomly distributed VO<sub>4</sub> units and scattered dangling oxygen bonds, which facilitated O–O binding. Moreover, a-LVOF demonstrates a high capacity of 230 mAh g<sup>−1</sup>. Our findings reveal a low-voltage O–O formal redox mechanism in an amorphized cathode material.</p>

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An amorphous Li–V–O–F cathode with tetrahedral coordination and O–O formal redox at low voltage

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月22日

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  • Kun Zhang,
  • Tonghuan Yang,
  • Tao Chen,
  • Yali Yang,
  • Zewen Jiang,
  • Chuan Gao,
  • Yuxuan Zuo,
  • Wukun Xiao,
  • Dingguo Xia

摘要

The ever-increasing demand for lithium-ion batteries has necessitated the development of high-performance cathode materials. However, previous studies have predominantly focused on crystal cathodes comprising the octahedral coordination of metal atoms and a well-ordered layered topology. This omits other cathode materials with other structures or coordination that could potentially surpass conventional counterparts in terms of performance. Here, using X-ray diffraction, resonant inelastic X-ray scattering and X-ray absorption near-edge spectra experiments, we investigated an amorphous Li–V–O–F cathode (a-LVOF) with tetrahedral coordination and elucidated an O–O formal redox mechanism at a moderate voltage of 4.1 V, without a conventional octahedral Li–O–Li configuration. The electrochemically amorphized material fosters randomly distributed VO4 units and scattered dangling oxygen bonds, which facilitated O–O binding. Moreover, a-LVOF demonstrates a high capacity of 230 mAh g−1. Our findings reveal a low-voltage O–O formal redox mechanism in an amorphized cathode material.