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Magnetic Field-induced Disordered Phase of Spinel Oxides for High Battery Performance.

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Summary

Local magnetic fields from Fe3O4 shells induce a disordered phase in lithium manganese nickel oxide (LNMO) cathodes at lower temperatures. This method enhances electrochemical performance and cycling stability without increasing detrimental Mn3+ content.

Keywords:
cycling stabilitylithium‐ion batterylocal magnetic fieldphase transitionradical pair mechanism

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • The disordered phase of spinel lithium manganese nickel oxide (LiMn1.5Ni0.5O4, LNMO) offers superior electrochemical performance for high-voltage cathodes compared to its ordered counterpart.
  • Current methods to induce this disordered phase often lead to capacity degradation due to increased Mn3+ content.

Purpose of the Study:

  • To investigate the use of local magnetic fields to induce a disordered phase transition in LNMO at lower temperatures.
  • To mitigate capacity degradation by minimizing the increase in Mn3+ content during the phase transition.

Main Methods:

  • Coating LNMO with a magnetic Fe3O4 shell to generate local magnetic fields.
  • Comparing phase transitions in LNMO with Fe3O4 shells, nonmagnetic Al2O3 shells, sole heat treatment, and heat treatment within magnetic fields.
  • Utilizing electrochemical characterization to evaluate performance, cycling stability, and kinetic properties.

Main Results:

  • Local magnetic fields effectively induced the order-disorder phase transition in LNMO at lower temperatures.
  • The presence of the magnetic Fe3O4 shell was crucial, unlike nonmagnetic Al2O3 shells or sole heat treatment.
  • The disordered LNMO with Fe3O4 shell demonstrated excellent cycling stability and improved kinetic properties.
  • Evidence suggests a radical pair mechanism initiated by magnetic fields drives the phase transition.

Conclusions:

  • Local magnetic fields can be a novel tool to control phase transitions in cathode materials like LNMO.
  • This approach enables the formation of disordered LNMO with enhanced electrochemical properties and reduced Mn3+ content.
  • The study highlights the potential of magnetic field effects in materials engineering for energy storage applications.