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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Conversion-type cathodes offer high energy density for lithium-ion batteries.
  • Sluggish nanoscale kinetics and complex phase transformations hinder their performance.
  • Copper fluoride (CuF2) cathodes historically suffer from irreversibility issues.

Purpose of the Study:

  • To reconcile the electrochemical reversibility of isostructural FeF2 and CuF2 cathodes.
  • To overcome the irreversibility limitations of CuF2 cathodes for improved lithium-ion battery performance.
  • To elucidate the role of interfacial kinetics in conversion reactions.

Main Methods:

  • Infiltration of liquid gallium (Ga) into a CuF2/carbon matrix to form a percolation network (pGa-CuF2/C).
  • Mechanistic studies to investigate the effect of Ga on fluorine mobility and phase transformations.
  • Fabrication of an optimized pGa-CuF2/C@TiO2 core-shell structure.

Main Results:

  • The Ga interlayer enabled reversible two-electron transfer via a displacement-reaction pathway in CuF2.
  • Ga retarded fluorine mobility, promoting the Li2CuF4 intermediate phase.
  • Ga minimized lattice mismatch and interfacial energy, facilitating homogeneous nucleation and a bicontinuous copper network.
  • The optimized core-shell structure achieved ~300 mAh/g at 2.8 V after 20 cycles.

Conclusions:

  • Interfacial kinetics are critical in determining the pathway and reversibility of conversion reactions.
  • Modulating interfacial energy and lattice mismatch is key to unlocking the potential of conversion cathodes.
  • Gallium infiltration presents a viable strategy to enhance the performance of fluoride-based conversion cathodes.