☆ 4.6 Article

Thermodynamic and spectroscopic properties of oxygen on silver under an oxygen atmosphere

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2015)

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 17, 期 14, 页码 9288-9312

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c5cp00342c

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Chemistry, Physical Physics, Atomic, Molecular & Chemical

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  1. CINECA award under the ISCRA initiative
  2. Australian Research Council

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We report on a combined density functional theory and the experimental study of the O-1s binding energies and X-ray Absorption Near Edge Structure (XANES) of a variety of oxygen species on Ag(111) and Ag(110) surfaces. Our theoretical spectra agree with our measured results for known structures, including the p(N x 1) reconstruction of the Ag(110) surface and the p(4 x 4) reconstruction of the Ag(111) surface. Combining the O-1s binding energy and XANES spectra yields unique spectroscopic fingerprints, allowing us to show that unreconstructed atomic oxygen is likely not present on either surface under equilibrium conditions at oxygen chemical potentials typical for ethylene epoxidation. Furthermore, we find no adsorbed or dissolved atomic species whose calculated spectroscopic features agree with those measured for the oxygen species believed to catalyze the partial oxidation of ethylene.

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