Surface oxidation of Pt and PtPd alloys during NO conversion investigated by Atom Probe Tomography

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Hauptverfasser: Lee, Yoonhee, Dobesch, Daniel, Stender, Patrick, Tuttlies, Ute, Nieken, Ulrich, Schmitz, Guido
Format: Preprint
Veröffentlicht: 2025
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author Lee, Yoonhee
Dobesch, Daniel
Stender, Patrick
Tuttlies, Ute
Nieken, Ulrich
Schmitz, Guido
author_facet Lee, Yoonhee
Dobesch, Daniel
Stender, Patrick
Tuttlies, Ute
Nieken, Ulrich
Schmitz, Guido
contents In this study, the dynamic oxidation state changes of pure Pt and 50at% PtPd alloy catalysts were investigated during a temperature ramp from 80 to 450 C under a reactive gas mixture of 500 ppm NO and 3 % Oxygen in Nitrogen atmosphere. These changes are closely correlated with variations in NO conversion efficiency. Sharp tip specimens were prepared from Pt and PtPd alloy wires by electrochemical polishing and Focused Ion Beam annular milling, with the hemispherical apex serving as a model for nanoscale catalyst surfaces. The samples were exposed to the reactive atmosphere in a dedicated reaction chamber and subsequently analyzed using atom probe tomography. Effective oxide thicknesses and three-dimensional surface morphology were quantitatively evaluated. A pronounced decrease in oxide thickness was observed during the first cooling and second heating cycles, particularly below 200 C, indicating reversible redox behavior on both Pt and PtPd alloy surfaces. This behavior correlates with the inverse hysteresis of NO conversion measured for both systems, suggesting that the redox reversibility is driven primarily by reaction kinetics rather than thermodynamic stability.
format Preprint
id arxiv_https___arxiv_org_abs_2511_23176
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Surface oxidation of Pt and PtPd alloys during NO conversion investigated by Atom Probe Tomography
Lee, Yoonhee
Dobesch, Daniel
Stender, Patrick
Tuttlies, Ute
Nieken, Ulrich
Schmitz, Guido
Materials Science
In this study, the dynamic oxidation state changes of pure Pt and 50at% PtPd alloy catalysts were investigated during a temperature ramp from 80 to 450 C under a reactive gas mixture of 500 ppm NO and 3 % Oxygen in Nitrogen atmosphere. These changes are closely correlated with variations in NO conversion efficiency. Sharp tip specimens were prepared from Pt and PtPd alloy wires by electrochemical polishing and Focused Ion Beam annular milling, with the hemispherical apex serving as a model for nanoscale catalyst surfaces. The samples were exposed to the reactive atmosphere in a dedicated reaction chamber and subsequently analyzed using atom probe tomography. Effective oxide thicknesses and three-dimensional surface morphology were quantitatively evaluated. A pronounced decrease in oxide thickness was observed during the first cooling and second heating cycles, particularly below 200 C, indicating reversible redox behavior on both Pt and PtPd alloy surfaces. This behavior correlates with the inverse hysteresis of NO conversion measured for both systems, suggesting that the redox reversibility is driven primarily by reaction kinetics rather than thermodynamic stability.
title Surface oxidation of Pt and PtPd alloys during NO conversion investigated by Atom Probe Tomography
topic Materials Science
url https://arxiv.org/abs/2511.23176