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Structure and Chemistry of Flat and Stepped Rh Surfaces during NO Dissociation near 1 mbar

García-Martínez, Fernando ; Sjö, Hanna LU ; Ali, Khadiza LU orcid ; Rämisch, Lisa LU ; Wallander, Harald LU ; Merte, Lindsay R. LU ; Hegedüs, Zoltan ; Zetterberg, Johan LU orcid ; Lundgren, Edvin LU and Schiller, Frederik , et al. (2026) In Journal of the American Chemical Society 148(14). p.14824-14834
Abstract

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... (More)

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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of the American Chemical Society
volume
148
issue
14
pages
11 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:41926652
  • scopus:105035915657
ISSN
0002-7863
DOI
10.1021/jacs.5c18969
language
English
LU publication?
yes
id
13cf69cc-5a3d-447a-bee4-2cd9a1ea3b76
date added to LUP
2026-05-19 15:15:44
date last changed
2026-07-16 02:05:45
@article{13cf69cc-5a3d-447a-bee4-2cd9a1ea3b76,
  abstract     = {{<p>The dissociation of NO is a critical step in its catalytic reduction to N<sub>2</sub>, 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.</p>}},
  author       = {{García-Martínez, Fernando and Sjö, Hanna and Ali, Khadiza and Rämisch, Lisa and Wallander, Harald and Merte, Lindsay R. and Hegedüs, Zoltan and Zetterberg, Johan and Lundgren, Edvin and Schiller, Frederik and Gustafson, Johan and Ortega, J. Enrique}},
  issn         = {{0002-7863}},
  language     = {{eng}},
  number       = {{14}},
  pages        = {{14824--14834}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Journal of the American Chemical Society}},
  title        = {{Structure and Chemistry of Flat and Stepped Rh Surfaces during NO Dissociation near 1 mbar}},
  url          = {{http://dx.doi.org/10.1021/jacs.5c18969}},
  doi          = {{10.1021/jacs.5c18969}},
  volume       = {{148}},
  year         = {{2026}},
}