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Modelling adsorbate coverage on complex alloy surfaces.

Martin L S Nielsen1, Jack K Pedersen1, Marcus F Nygaard1

  • 1Center for High Entropy Alloy Catalysis (CHEAC), Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen, Denmark. jan.rossmeisl@chem.ku.dk.

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New rules for adsorbate interactions simplify catalysis theory for complex alloys. For Palladium-Silver (PdAg) alloys, these rules predict improved oxygen reduction reaction activity due to adsorbed hydroxyl (*OH) species.

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Area of Science:

  • Materials Science
  • Theoretical Chemistry
  • Surface Science

Background:

  • Extending catalysis theory to complex alloys and multiple adsorbates is computationally challenging due to numerous surface site-adsorbate combinations.
  • Existing models often struggle to accurately predict adsorbate behavior on alloy surfaces.

Purpose of the Study:

  • To develop a simplified approach for catalysis theory applicable to complex alloys and multiple adsorbates.
  • To investigate the impact of adsorbate-adsorbate interaction rules on surface coverage and catalytic activity.
  • To predict the performance of Palladium-Silver (PdAg) alloys in the oxygen reduction reaction.

Main Methods:

  • Defining blocking rules for disallowed local adsorbate-adsorbate configurations.
  • Conducting simple simulations to test the effect of different interaction rules.
  • Applying the simulation approach to PdAg intermetallic and solid solutions, and to Ag14Ir16Pd30Pt14Ru26 high-entropy alloys.

Main Results:

  • In PdAg alloys, Silver (Ag) atoms prevent full oxygen (O*) coverage, allowing adsorbed hydroxyl (*OH) species formation.
  • Adsorbed *OH species are predicted to enhance oxygen reduction reaction activity, reaching optimal adsorption energies.
  • The influence of interaction rules on oxygen reduction was less distinct in high-entropy alloys compared to binary PdAg alloys.

Conclusions:

  • The developed adsorbate-adsorbate interaction rules provide a viable method for studying complex alloy catalysis.
  • The findings offer experimental guidance for distinguishing PdAg(111) alloy surface structures and understanding adsorbate coverage.
  • The approach highlights the potential of *OH species for improving oxygen reduction reaction activity in PdAg systems.