Structure and Chemistry of Flat and Stepped Rh Surfaces during NO Dissociation near 1 mbar
Artikel i vetenskaplig tidskrift, 2026
The dissociation of NO is a critical step in its catalytic reduction to N2, which is key to automotive exhaust treatment. Here, we examine the role of Rh atomic steps in the NO dissociation reaction under 0.05 mbar NO. We use a Rh crystal sample curved around the (111) direction and ambient-pressure X-ray photoelectron spectroscopy to probe different Rh surfaces subject to the very same reaction conditions. At the dissociation onset, this approach allows us to quantitatively determine the NO species involved in the reaction, and to rationally assess the process in terms of diffusion and dissociation probability at terraces and steps. At a higher temperature we trigger surface oxidation, which begins preferentially on flat Rh(111) and B-type stepped surfaces, as compared to A-type stepped surfaces. Surface X-ray diffraction performed on single crystal samples reveals similar oxide structures at the atomic scale, but while B-type Rh(553) and Rh(111) surfaces do not reconstruct, A-type Rh(223) facet exhibits faceting. These findings underscore the structural sensitivity of NO dissociation and its potential impact on Rh-catalyzed NO reduction.
Författare
Fernando Garcia-Martinez
Universidad del Pais Vasco / Euskal Herriko Unibertsitatea
Deutsches Elektronen-Synchrotron (DESY)
Hanna Sjo
Lunds universitet
Khadiza Ali
Chalmers, Mikroteknologi och nanovetenskap, Kvantkomponentfysik
Lisa Ramisch
Lunds universitet
Harald Wallander
Lunds universitet
Malmö universitet
Lindsay R. Merte
Malmö universitet
Lunds universitet
Zoltan Hegedus
Deutsches Elektronen-Synchrotron (DESY)
Johan Zetterberg
Lunds universitet
Edvin Lundgren
Lunds universitet
Frederik Schiller
Universidad del Pais Vasco / Euskal Herriko Unibertsitatea
Johan Gustafson
Lunds universitet
J. Enrique Ortega
Universidad del Pais Vasco / Euskal Herriko Unibertsitatea
Journal of the American Chemical Society
0002-7863 (ISSN) 1520-5126 (eISSN)
Vol. 148 14824-14834Kähler-Einstein metrics, random point processes and variational principles (RANDOM-KAHLER)
Europeiska kommissionen (EU), 2013-01-01 -- 2017-12-31.
Europeiska kommissionen (EU), 2013-01-01 -- 2017-12-31.
Atomär design av katalysatorer
Knut och Alice Wallenbergs Stiftelse (KAW2015.0058), 2016-01-07 -- 2021-06-30.
Ämneskategorier (SSIF 2025)
Atom- och molekylfysik och optik
Oorganisk kemi
Fysikalisk kemi
DOI
10.1021/jacs.5c18969
PubMed
41926652