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CO adsorption and dissociation on “perfect” and “defect-rich” Ir(111) surfaces were studied by a combination of surface-analytical techniques, including polarization-dependent (PPP and SSP) sum frequency generation (SFG) vibrational spectroscopy, low-energy electron diffraction (LEED), Auger electron spectroscopy, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. CO was found to be ordered and tilted from the surface normal at high coverage on the “perfect” surface (e.g., θ = 30° at 0.70 ML), whereas it was less ordered and preferentially upright (θ = 4–10°) on the “defect-rich” surface for coverages of 0.55–0.70 ML. SFG, LEED, and XPS revealed that CO adsorption at low pressure/high temperature and high pressure/low temperature was reversible. In contrast, upon heating to ∼600 K in near mbar CO pressure, “perfect” and even more “defect-rich” Ir(111) surfaces were irreversibly modified by carbon deposits, which, according to DFT, result from CO disproportionation.

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