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Area of Science:

  • Electrochemistry
  • Chemical Engineering
  • Materials Science

Background:

  • Coupled electron- and phase-transfer reactions are vital for electrochemical energy conversion and storage.
  • Understanding their mechanism, energetics, and kinetics is key to improving device performance.

Purpose of the Study:

  • To develop and demonstrate an experimental methodology for quantitatively investigating coupled electron- and phase-transfer reactions at an individual, well-defined three-phase interface.
  • To elucidate the behavior of ferrocene oxidation and ferrocenium transfer across a liquid-liquid interface.

Main Methods:

  • Utilized a Pt-Ir wire electrode positioned across a water/1,2-dichloroethane interface to create a defined three-phase boundary.
  • Employed cyclic voltammetry to study ferrocene oxidation and ferrocenium transfer.
  • Applied finite-element simulations to model the electrochemical response.

Main Results:

  • Observed distinct reversible waves for ferrocene oxidation and ferrocenium reduction/reoxidation in cyclic voltammetry.
  • Demonstrated that ferrocenium transfer into the aqueous phase is influenced by electrolyte concentration, peaking at intermediate concentrations.
  • Simulations confirmed the localized nature of the electrochemical response near the interface.

Conclusions:

  • The developed methodology allows for quantitative investigation of coupled electron and phase transfer at a three-phase boundary.
  • The rate of ion transfer across the interface is significantly affected by the electric field distribution, influenced by electrolyte concentration.
  • This work provides fundamental insights into processes critical for electrochemical energy devices.