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1.
Angew Chem Int Ed Engl ; 59(45): 20037-20043, 2020 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-32701180

RESUMEN

The catalytic oxidation of CO on transition metals, such as Pt, is commonly viewed as a sharp transition from the CO-inhibited surface to the active metal, covered with O. However, we find that minor amounts of O are present in the CO-poisoned layer that explain why, surprisingly, CO desorbs at stepped and flat Pt crystal planes at once, regardless of the reaction conditions. Using near-ambient pressure X-ray photoemission and a curved Pt(111) crystal we probe the chemical composition at surfaces with variable step density during the CO oxidation reaction. Analysis of C and O core levels across the curved crystal reveals that, right before light-off, subsurface O builds up within (111) terraces. This is key to trigger the simultaneous ignition of the catalytic reaction at different Pt surfaces: a CO-Pt-O complex is formed that equals the CO chemisorption energy at terraces and steps, leading to the abrupt desorption of poisoning CO from all crystal facets at the same temperature.

2.
J Synchrotron Radiat ; 26(Pt 4): 1288-1293, 2019 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-31274456

RESUMEN

Platinum thin films activated ex situ by oxygen plasma become reduced by the combined effect of an intense soft X-ray photon beam and condensed water. The evolution of the electronic structure of the surface has been characterized by near-ambient-pressure photoemission and mimics the inverse two-step sequence observed in the electro-oxidation of platinum, i.e. the surface-oxidized platinum species are reduced first and then the adsorbed species desorb in a second step leading to a surface dominated by metallic platinum. The comparison with measurements performed under high-vacuum conditions suggests that the reduction process is mainly induced by the reactive species generated by the radiolysis of water. When the photon flux is decreased, then the reduction process becomes slower.

4.
J Synchrotron Radiat ; 22(6): 1528-30, 2015 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-26524318

RESUMEN

A 30 µm pinhole is introduced in the intermediate focus of the SIM beamline at the Swiss Light Source to improve the spot size at the second downstream focus, which is used here for liquid jet X-ray photoelectron spectroscopy experiments. The 30 µm pinhole reduces the beam dimensions from 250 (v) × 100 (h) µm to 75 × 45 µm for a vertical exit slit of 100 µm. The smaller X-ray spot results in a substantial decrease in the gas-phase contribution of the spectra from 40% down to 20% and will help to simplify the interpretation and peak assignments of future experiments.

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