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CO Adsorption and Disproportionation on Smooth and Defect-Rich Ir(111).

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The Journal of Physical Chemistry. C, Nanomaterials and Interfaces
|May 2, 2022
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Carbon monoxide (CO) adsorption on iridium surfaces differs based on surface defects. Defects lead to upright CO, while perfect surfaces show tilted CO, with both reversible under certain conditions.

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Area of Science:

  • Surface Science
  • Physical Chemistry
  • Materials Science

Background:

  • Understanding CO adsorption on transition metal surfaces is crucial for catalysis.
  • Iridium (Ir) surfaces are important in various catalytic processes.
  • Surface defects can significantly alter adsorption behavior.

Purpose of the Study:

  • To investigate the adsorption and dissociation of CO on perfect and defect-rich Ir(111) surfaces.
  • To compare the structural and electronic properties of CO on these surfaces.
  • To elucidate the mechanisms of CO adsorption, desorption, and surface modification.

Main Methods:

  • Sum frequency generation (SFG) vibrational spectroscopy (polarization-dependent PPP and SSP).
  • Low-energy electron diffraction (LEED), Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS).
  • Density functional theory (DFT) calculations.

Main Results:

  • CO adsorbs tilted (∼30°) on perfect Ir(111) at high coverage, but upright (4-10°) on defect-rich surfaces.
  • CO adsorption is reversible under low pressure/high temperature or high pressure/low temperature conditions.
  • Irreversible surface modification by carbon deposits occurs upon heating to ~600 K in mbar CO, attributed to CO disproportionation.

Conclusions:

  • Surface defects on Ir(111) promote upright CO adsorption and influence its ordering.
  • CO adsorption/desorption is reversible, but high temperature/pressure can lead to irreversible carbon formation.
  • CO disproportionation is identified as the mechanism for carbon deposit formation on Ir(111).