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Nick D'Antona1,2, Joseph Kelly3, Nadia Barnard1

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This study quantifies proton transfer kinetics at liquid|liquid interfaces using facilitated proton transfer. Researchers measured key kinetic parameters, revealing direct proton transfer is favored under specific conditions.

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Area of Science:

  • Electrochemistry
  • Physical Chemistry
  • Chemical Engineering

Background:

  • Proton transfer is crucial for electrochemical processes but difficult to measure at electrode interfaces.
  • Existing methods are complicated by electron transfer and surface defects.
  • The interface between two immiscible electrolyte solutions (ITIES) offers a simplified system.

Purpose of the Study:

  • To investigate proton transfer kinetics at the ITIES, free from electron transfer and surface irregularities.
  • To establish a model system for studying fundamental proton transfer mechanisms.
  • To determine kinetic parameters for facilitated proton transfer.

Main Methods:

  • Utilized diffusion-controlled micropipette voltammetry and nanopipette-supported interfaces.
  • Employed a mixed diffusive-kinetic model to analyze voltammograms.
  • Performed finite-element and atomistic molecular-dynamics simulations.

Main Results:

  • 2,6-diphenylpyridine (DPP) was identified as a facilitator for proton transfer across the HCl(aq)|trifluorotoluene interface.
  • Apparent kinetic parameters (k°app = 3.0 ± 1.8 cm/s, αapp = 0.3 ± 0.2) were extracted.
  • Simulations indicated a preference for direct proton transfer when DPP partitioning was rate-limiting.
  • Molecular dynamics predicted proton transfer occurs in the interpenetrating liquid surface region.

Conclusions:

  • The ITIES platform provides a robust method for studying intrinsic proton transfer kinetics.
  • Understanding ion transfer at ITIES contributes to broader theories in electrochemical science.
  • This research offers insights into facilitated proton transfer mechanisms and interfacial phenomena.