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Fluid-enhanced surface diffusion controls intraparticle phase transformations.

Yiyang Li1,2,3, Hungru Chen4, Kipil Lim1,5

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Lithium ions migrate along particle surfaces in LiXFePO4 batteries, enhancing conductivity. This fluid-enhanced surface diffusion is key to controlling phase transformations in anisotropic materials.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Phase transformations in anisotropic solids like LiXFePO4 (lithium iron phosphate) are crucial for battery performance.
  • Poor bulk ionic transport along specific crystallographic directions hinders efficient lithium-ion (Li+) migration during these transformations.

Purpose of the Study:

  • To elucidate the mechanism of lithium ion migration during phase transformations in LiXFePO4.
  • To investigate the role of surface diffusion and fluid interactions in overcoming transport limitations.

Main Methods:

  • X-ray diffraction and microscopy experiments.
  • Ab initio molecular dynamics simulations.
  • Phase-field simulations.

Main Results:

  • Lithium ions migrate along the solid/liquid interface within particles, not requiring bulk transport or crossing the double layer.
  • Organic solvents and water molecules significantly enhance surface ion diffusion, enabling effective 3D Li+ conduction.
  • Phase-field simulations confirmed the impact of surface diffusion on phase transformation dynamics.

Conclusions:

  • Fluid-enhanced surface diffusion is a critical mechanism for lithium ion transport in anisotropic materials like LiXFePO4.
  • Controlling surface diffusivity offers a new strategy to tune and suppress undesirable phase separation in battery electrodes.
  • This finding redefines LiXFePO4 as a 3D lithium-ion conductor through surface-mediated transport.