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Surface acidity in heterogeneous metal oxides is crucial for water oxidation catalysis. This study reveals how pH influences intermediates, linking surface acidity to catalytic mechanisms and hydration layer effects.

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Area of Science:

  • Surface Chemistry
  • Catalysis
  • Photochemistry

Background:

  • Protonation of homogeneous metal-oxide catalysts is understood, but surface acidity's role in heterogeneous metal oxides remains unclear.
  • Current understanding of surface acidity is limited to rationalizing pH-dependent product evolution due to a lack of metrics for transient intermediates.

Purpose of the Study:

  • To investigate the pH dependence of metastable intermediates in water oxidation catalysis.
  • To establish a link between surface acidity and the chemical steps of water oxidation at a heterogeneous metal oxide interface.

Main Methods:

  • Utilized time-resolved visible broadband probe spectroscopy to detect emissive intermediates.
  • Studied photoexcitation of the oxygen evolution reaction (OER) at an electron-doped SrTiO3/aqueous interface.
  • Analyzed the pH dependence of intermediate populations over their entire lifetime (<2 ps to 10 μs).

Main Results:

  • The pH dependence of a transient intermediate population (<2 ps) was preserved as it decayed over 10 μs, with a pH onset at 11.4.
  • A distinct surface acidity was ascribed to the first water oxidation intermediate, with a pKa indicating a transition between Ti-OH• and Ti-O•- species.
  • Excited state optical spectroscopy proved sensitive to protonation of metastable intermediates.

Conclusions:

  • Surface acidity plays a critical role in the mechanism of water oxidation catalysis at heterogeneous metal oxide interfaces.
  • The hydration layer's properties significantly influence the stability of intermediates with varying acidities, impacting subsequent catalytic steps.
  • This work highlights the utility of excited state spectroscopy in probing proton transfer dynamics in catalytic systems.