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Area of Science:

  • Materials Science
  • Electrochemistry
  • Surface Science

Background:

  • Polarons significantly influence semiconductor (photo)electrocatalytic performance.
  • Conventional polaron introduction is irreversible and occurs during synthesis.

Purpose of the Study:

  • To develop an in situ, reversible method for polaron formation using external electrode potential.
  • To investigate the impact of potential-dependent polarons on the hydrogen evolution reaction (HER) on TiO2.

Main Methods:

  • Combined grand canonical ensemble density functional theory (DFT) calculations.
  • (In situ spectro) electrochemical experiments.

Main Results:

  • Demonstrated potential-dependent polaron formation (Ti4+ to Ti3+ surface polarons) in TiO2 at reducing potentials.
  • Observed significant changes in TiO2 electronic structure.
  • Identified potential-dependent polarons as highly active sites for HER, altering adsorption energy relationships and reaction kinetics.

Conclusions:

  • In situ polaron generation can be strategically used to enhance semiconductor (photo)electrode performance.
  • Provided atomistic insights into potential-dependent polaron formation in electrocatalysis.