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Area of Science:

  • Electrochemistry
  • Materials Science

Background:

  • Hematite is a promising material for oxygen evolution reaction (OER) electrocatalysis.
  • Understanding the reaction mechanism, particularly the rate-determining step, is crucial for improving OER efficiency.
  • The oxygen evolution reaction is vital for energy conversion technologies like water splitting.

Purpose of the Study:

  • To investigate the effect of pyridine derivatives on the OER mechanism on hematite electrodes.
  • To determine if concerted proton-coupled electron transfer (CPET) can be induced and if it impacts the reaction kinetics.
  • To quantify the change in overpotential for OER at neutral pH.

Main Methods:

  • Electrochemical measurements were performed on hematite electrodes.
  • Pyridine derivatives were added to the electrolyte to modify the reaction pathway.
  • Kinetic analysis was used to identify the rate-determining step of the OER.

Main Results:

  • The addition of pyridine derivatives shifted the rate-determining step from sequential electron/proton transfer to CPET.
  • Inducing the CPET process resulted in a significant decrease in overpotential for OER.
  • The overpotential for oxygen evolution at neutral pH was reduced by approximately 250 mV.

Conclusions:

  • Pyridine derivatives can effectively promote CPET in the OER on hematite.
  • Switching to a CPET mechanism offers a viable strategy for reducing the overpotential and enhancing OER efficiency.
  • This finding has implications for the development of more efficient electrocatalysts for water oxidation.