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Characterization of Electrode Materials for Lithium Ion and Sodium Ion Batteries Using Synchrotron Radiation Techniques
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Structural Evolution in Disordered Rock Salt Cathodes.

Tianyu Li1,2, Tullio S Geraci3,4, Krishna Prasad Koirala5,6

  • 1Materials Department, University of California Santa Barbara, Santa Barbara 93106, California, United States.

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|August 22, 2024
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Summary
This summary is machine-generated.

Li-excess disordered rock salt oxides (DRX) transform into a beneficial "δ phase" upon heating, enhancing Li-ion battery capacity. This structural evolution, driven by cation migration, is more pronounced in manganese-rich materials.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Li-excess disordered rock salt oxides (DRX) are cost-effective cathode materials for Li-ion batteries with high theoretical capacities.
  • Mn-rich DRX (Li1+MnM1-O2, y ≥ 0.5) show capacity increases during cycling, linked to the formation of a "δ phase" with spinel-like domains.

Purpose of the Study:

  • To systematically investigate the structural evolution of Mn-based DRX upon heating at various delithiation states.
  • To understand the structural rearrangements during battery cycling and the mechanism of "δ phase" formation.

Main Methods:

  • Synchrotron X-ray and neutron diffraction to analyze the structure of the "δ phase".
  • In situ heating X-ray diffraction (XRD) experiments.
  • Thermochemical studies.

Main Results:

  • All studied DRX structures relax to the "δ phase" upon heating, leading to capacity enhancement.
  • Selective Li and Mn/Ti cation migration within the DRX structure causes the observed structural rearrangements.
  • Both Mn-rich and Mn-poor DRX can relax to the "δ phase" after delithiation, but with different domain structures.

Conclusions:

  • The "δ phase" formation is a key mechanism for capacity enhancement in Li-excess Mn-based DRX.
  • Mn-rich DRX exhibits a greater thermodynamic driving force and lower activation energy for "δ phase" relaxation, explaining its prevalence during battery cycling.