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Area of Science:

  • Electrochemistry
  • Catalysis
  • Physical Chemistry

Background:

  • Electrocatalysts can create localized microenvironments with pH distinct from the bulk solution.
  • These local pH changes significantly affect proton-coupled electron transfer reactions, influencing energy efficiency and selectivity.
  • Studies have characterized local pH in reductive reactions, but oxidative reactions like oxygen evolution reaction (OER) remain less explored due to technical challenges.

Purpose of the Study:

  • To develop a predictive model for local pH gradients as a function of current density.
  • To experimentally observe and validate pH gradient formation and dissipation during OER.
  • To provide insights into catalyst design for improved energy conversion efficiency.

Main Methods:

  • A model was developed using bulk pH, buffer composition, pKa, and mass transport parameters.
  • An acid-stable lead oxide (PbO2) electrocatalyst was used for oxygen evolution reaction (OER) studies.
  • Voltammetric and potentiometric measurements were employed to validate the model and observe pH gradients.

Main Results:

  • The model successfully describes local pH as a function of current density, independent of specific reaction mechanisms.
  • Experimental observations confirmed the formation and dissipation of pH gradients during OER.
  • A narrow OER current density window was identified where local acidic environments can develop.

Conclusions:

  • The developed model accurately predicts local pH gradients in electrocatalytic reactions.
  • The findings highlight the importance of acid-stable catalysts for OER, even in basic media.
  • The model is broadly applicable to various electrocatalytic reactions involving proton generation or consumption in energy conversion.