Crowded electrolytes containing redoxmers in different states of charge: solution structure and properties

(a) Li+ ion interacting with phenothiazine, (b) A gel-like solution of phenothiazine in electrolyte, (c) dependence of solvent diffusivity vs. molarity of neutral and charged redoxmer.

Scientific Achievement

Neutral and charged crowded electrolytes containing redox active organic molecules (redoxmers) are shown to suffer exponential decline in their dynamic properties as they approach the gel-like regime that sets in between 1 and 2 M.

Significance and Impact

In crowded all-organic electrolyte solutions there are hard limits for increasing energy density that cannot be surpassed regardless of the redoxmer nature or electrolyte composition. Only select systems in hot ionic liquid like solutions can have favorable dynamic properties  allowing 2.5-3 M operation of electrochemical cells.

Research Details

  • Phenothiazine redoxmers miscible with acetonitrile based electrolyte were used to study crowding effects
  • Viscosity, ionic conductivity, diffusivity, and x-ray scattering were studied
  • Liquid-like and gel like behaviors were observed and rationalized using molecular dynamics modeling.

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