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Evaluation of Interfacial pH Using Surface Forces Apparatus Fluorescence Spectroscopy.

Motohiro Kasuya1, Yuka Sano1, Masataka Kawashima1

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Interfacial pH near surfaces is influenced by electrolyte concentration and type, and substrate material. Simple electric double layer theory explains some effects, but ion adsorption and substrate chemistry also play key roles.

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Area of Science:

  • Physical Chemistry
  • Surface Science
  • Electrochemistry

Background:

  • Understanding interfacial pH is crucial for various chemical and biological processes.
  • Surface Force Apparatus (SFA) fluorescence spectroscopy offers a unique method to probe these phenomena.
  • Previous studies have not fully elucidated the factors governing interfacial pH in confined geometries.

Purpose of the Study:

  • To investigate the interfacial pH of aqueous electrolytes confined between surfaces.
  • To determine the influence of electrolyte concentration, cationic species, and substrate material on interfacial pH.
  • To differentiate between the contributions of the electric double layer (EDL) effect and other factors.

Main Methods:

  • Utilized Surface Force Apparatus (SFA) fluorescence spectroscopy with a pH probe (C. SNARF-4F).
  • Measured interfacial pH as a function of surface separation (D) for various aqueous electrolyte concentrations and cationic species (Cs+, Na+, Li+).
  • Performed electric double layer (EDL) model calculations based on SFA-derived surface potentials.

Main Results:

  • Interfacial pH of aqueous CsCl between mica decreased exponentially with decreasing surface separation.
  • EDL model accurately predicted interfacial pH at low electrolyte concentrations (0.1 mM).
  • At higher concentrations (0.4-10 mM), measured pH deviated from EDL predictions, indicating additional influencing factors.
  • Interfacial pH was found to depend on electrolyte concentration, species, and substrate (mica vs. silica).

Conclusions:

  • Interfacial pH is not solely governed by the general EDL effect, especially at higher electrolyte concentrations.
  • Ion adsorption at the interface and the chemical states of the substrates significantly impact interfacial pH.
  • These findings highlight the complexity of interfacial electrochemistry in confined systems.