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Exploring dynamic solvation kinetics at electrocatalyst surfaces.

Francisco Sarabia1, Carlos Gomez Rodellar1, Beatriz Roldan Cuenya1

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|September 18, 2024
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This summary is machine-generated.

Electrocatalyst interfaces are dynamic, with solvent and intermediate coverage changing over time and potential. Accounting for these dynamic effects is crucial for accurate kinetic models in reactions like hydrogen evolution and ammonia oxidation.

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Area of Science:

  • Electrocatalysis
  • Surface Science
  • Physical Chemistry

Background:

  • The electrocatalyst-electrolyte interface is highly dynamic, with intermediate coverage and interfacial solvent properties being bias and time-dependent.
  • Current kinetic models often overlook these dynamic interfacial phenomena, potentially limiting their predictive accuracy.

Purpose of the Study:

  • To investigate the kinetics of hydrogen evolution, ammonia oxidation, and oxygen reduction reactions on polycrystalline platinum.
  • To explore the influence of dynamic interfacial solvent and charged intermediates on reaction kinetics.
  • To elucidate the impact of pH on overpotential shifts and activation entropy.

Main Methods:

  • Studied kinetics of key electrochemical reactions on polycrystalline Pt.
  • Analyzed dynamic interfacial changes with millisecond time resolution.
  • Investigated electrosorption, double-layer charging, and catalyst poisoning effects (*N, *NO).

Main Results:

  • Discovered shared relationships between pre-exponential factor and activation energy, linked to solvation kinetics.
  • Observed bias and time-dependent kinetic parameters, including dynamic poisoning effects.
  • Identified pH-dependent activation entropy explaining non-Nernstian overpotential shifts.

Conclusions:

  • Dynamic interfacial solvent and surface properties significantly influence electrocatalytic kinetics.
  • Accurate kinetic models must incorporate bias and time-dependent interfacial phenomena.
  • Understanding these dynamics is key for optimizing electrocatalyst performance.