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Gas-Liquid-Solid Three-Phase Boundary in Scanning Electrochemical Cell Microscopy.

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Scanning electrochemical cell microscopy (SECCM) with gas transfer analysis enables precise electrochemical measurements. This study quantifies interfacial gas transfer effects, crucial for fuel cells and electrolyzers.

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Energy Conversion

Background:

  • The gas-liquid-solid interface is critical for electrochemical energy devices like fuel cells and electrolyzers.
  • Understanding gas transfer effects at this three-phase boundary is a significant challenge.
  • Scanning electrochemical cell microscopy (SECCM) offers a method to map electrochemical heterogeneity, inherently involving a three-phase boundary.

Purpose of the Study:

  • To quantitatively analyze the role of the three-phase boundary in gas-involved SECCM using finite element simulations.
  • To elucidate how interfacial gas transfer impacts electrochemical reactions.
  • To provide a basis for advanced SECCM applications in studying gas-involved electrochemistry.

Main Methods:

  • Finite element simulation was employed to model gas transfer at the three-phase boundary.
  • Oxygen reduction reaction was simulated as a case study for gas reactants.
  • Hydrogen evolution reaction was simulated as a case study for gas products.

Main Results:

  • Interfacial gas transfer enhances reactant mass transport, enabling high current density measurements (A/cm²).
  • Fast interfacial gas transfer for gas products minimizes dissolved gas concentration, facilitating high-current kinetic studies without bubble issues.
  • The contribution of interfacial gas transfer can be directly compared to solution mass transfer coefficients.

Conclusions:

  • Interfacial gas transfer significantly influences SECCM measurements involving gases.
  • This work establishes a quantitative framework for applying SECCM to gas-involved electrochemical reactions.
  • The findings support the investigation of electrochemistry at the three-phase boundary.