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Oxygen-Loss-Induced Structural Degradation in ε-LiVOPO4.

Hanlei Zhang1,2,3, Hui Zhou2, Zhi Deng4

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|December 20, 2022
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Summary
This summary is machine-generated.

Lattice oxygen loss in ε-LiVOPO₄ cathodes causes structural degradation. Mild oxygen loss induces reversible phase transformation, while higher temperatures lead to irreversible damage, offering insights for cathode design.

Keywords:
TEMbatterydegradationoperandooxygenphase transformation

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • ε-LiVOPO₄ is a promising cathode material for lithium-ion batteries due to its high capacity.
  • Structural degradation caused by oxygen loss is a critical issue for cathode performance but remains understudied.
  • Understanding oxygen loss mechanisms is crucial for developing stable and durable battery materials.

Purpose of the Study:

  • To investigate the atomic-scale mechanisms of lattice oxygen loss in ε-LiVOPO₄ cathodes.
  • To reveal the structural dynamics and phase transformation pathways induced by oxygen loss.
  • To explore strategies for mitigating structural degradation in oxide cathodes.

Main Methods:

  • Utilized *in situ* environmental transmission electron microscopy (ETEM) to observe structural changes at the atomic scale.
  • Spatially and temporally resolved lattice oxygen loss and phase transformations.
  • Investigated the effects of varying temperatures (400 °C, 500 °C, 600 °C) on structural integrity.

Main Results:

  • Mild oxygen loss at 400 °C triggered a reversible topotactic phase transformation (ε-LiVOPO₄ → α-Li₃V₂(PO₄)₃) via nucleation and growth, forming a core-shell structure.
  • Reversible transformation was achieved by switching to an oxidizing environment.
  • Severe oxygen loss at 500 °C and 600 °C resulted in irreversible structural damage, including amorphization and nanocavity formation due to high oxygen vacancy concentration.

Conclusions:

  • Demonstrated that oxygen loss is a key factor in the structural degradation of ε-LiVOPO₄ cathodes.
  • Identified distinct degradation mechanisms at different temperatures, highlighting the role of oxygen vacancies.
  • Proposed that controlling environmental conditions can be a strategy to manage structural stability and enhance cathode performance.