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Slab-Gliding-Induced Structural Evolution in β‑V2O5 Enables Reversible High Na-Ion Storage: A Combined Operando

Rafael Córdoba1, Jakub Goclon2, Angelina Sarapulova3,4,5

  • 1Departamento de Química y Bioquímica, Facultad de Farmacia, Universidad San Pablo-CEU, CEU Universities, Urbanización Montepríncipe, Boadilla del Monte, Madrid 28668, Spain.

Chemistry of Materials : a Publication of the American Chemical Society
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High-pressure beta-vanadium pentoxide (β-V2O5) shows promise for sodium-ion batteries. This study clarifies its reversible sodium intercalation mechanism through advanced techniques, revealing a unique phase transition sequence.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • High-pressure β-V2O5 is a promising cathode material for sodium-ion batteries, offering high capacity.
  • The exact mechanism of sodium intercalation and the resulting structural changes remain unclear.

Purpose of the Study:

  • To comprehensively investigate the structural evolution, oxidation state, and local structural changes of β-V2O5 during sodium intercalation.
  • To elucidate the reversible sodium (de)-intercalation mechanism in β-V2O5.

Main Methods:

  • Operando synchrotron X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS).
  • X-ray photoelectron spectroscopy (XPS) and ex situ transmission electron microscopy (TEM).
  • First-principles density functional theory (DFT) calculations.

Main Results:

  • Confirmed the reversibility of sodium (de)-intercalation in β-V2O5.
  • Determined the crystal structure of sodiated phases (NaxV2O5, 0 ≤ x ≤ 1) during cycling.
  • Identified a reversible phase transition sequence (P21/m → C2/m → P21/m) driven by V2O5 slab gliding.

Conclusions:

  • The sodium storage mechanism in β-V2O5 involves reversible phase transitions facilitated by layer gliding.
  • This provides a fundamental understanding of the electrochemical behavior of β-V2O5 for sodium-ion battery applications.