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Altering CO binding on gold cluster cations by Pd-doping.

Heider A Abdulhussein1, Piero Ferrari, Jan Vanbuel

  • 1School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT, UK. r.l.johnston@bham.ac.uk.

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|August 22, 2019
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Summary
This summary is machine-generated.

Doping gold clusters with palladium enhances carbon monoxide (CO) adsorption energy in a size-dependent manner. The binding site, either on gold or palladium atoms, influences CO vibrational frequency and electronic interactions.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Nanotechnology

Background:

  • Dopant atoms in metal nanoparticles modify interactions with adsorbates, crucial for catalysis.
  • Controlling adsorbate-metal interactions at the atomic level is key to designing efficient catalysts.

Purpose of the Study:

  • To investigate the influence of palladium (Pd) doping on the adsorption of carbon monoxide (CO) onto small cationic gold (AuN+) clusters.
  • To understand the atomic-level interactions governing CO binding on doped gold clusters.

Main Methods:

  • Combined experimental techniques: low-pressure collision cell reactivity and infrared multiple photon dissociation spectroscopy.
  • Theoretical calculations using density functional theory (DFT) to model cluster-CO interactions.

Main Results:

  • Pd doping increases CO adsorption energy on AuN+ clusters, with a size-dependent effect.
  • CO adsorption occurs on Au atoms for smaller doped clusters (N=3-5, 11) and on Pd dopants for larger clusters (N=6-10, 12-14).
  • Vibrational frequency shifts indicate electron charge transfer: red-shifting for Pd-CO interaction (back-donation) and blue-shifting for Au-CO interaction (σ-donation).

Conclusions:

  • Palladium doping significantly alters CO binding energies and sites on gold clusters.
  • The study provides atomic-level insights into adsorbate-dopant-host interactions in sub-nanometer metal clusters.
  • Understanding these fundamental interactions is vital for advancing heterogeneous catalysis research.