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Mixing plastic crystals like succinonitrile with other nitriles significantly boosts ionic conductivity, crucial for solid-state electrolytes in batteries. This study explores new mixtures and their conductivity enhancement mechanisms.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Electrochemistry

Background:

  • Plastic crystals exhibit high ionic conductivity, making them suitable for solid-state electrolytes.
  • Mixing plastic crystalline materials can enhance ionic conductivity, but few mixtures have been studied.
  • Succinonitrile is a prominent plastic-crystalline ionic conductor often used in mixtures.

Purpose of the Study:

  • To investigate the effect of mixing succinonitrile with malononitrile, adiponitrile, and pimelonitrile on ionic conductivity.
  • To examine the phase behavior and dynamics of these mixtures.
  • To understand the mechanism behind mixing-induced conductivity enhancement.

Main Methods:

  • Differential scanning calorimetry (DSC) to analyze phase behavior.
  • Dielectric spectroscopy to study molecular and ionic dynamics.
  • Ionic conductivity measurements.

Main Results:

  • The study examined succinonitrile mixed with malononitrile, adiponitrile, and pimelonitrile, with 1 mol.% Li ions added.
  • Mixing-induced enhancement of ionic conductivity was observed.
  • A coupling between translational ionic mobility and molecular reorientational dynamics was identified, likely via a revolving-door mechanism.

Conclusions:

  • Mixing succinonitrile with other nitriles can significantly enhance ionic conductivity.
  • The revolving-door mechanism is a probable explanation for the enhanced ionic mobility.
  • These findings support the potential of plastic crystal mixtures as advanced solid-state electrolytes.