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The structure-function relationship for alumina supported platinum during the formation of ammonia from nitrogen oxide and hydrogen in the presence of oxygen

Adams, Emma Catherine ; Merte, Lindsay Richard LU ; Hellman, Anders ; Skoglundh, Magnus ; Gustafson, Johan LU ; Bendixen, Eva Charlotte ; Gabrielsson, Pär ; Bertram, Florian LU ; Evertsson, Jonas LU and Zhang, Chu LU , et al. (2016) In Physical Chemistry Chemical Physics 18(16). p.10850-10855
Abstract

We study the structure-function relationship of alumina supported platinum during the formation of ammonia from nitrogen oxide and dihydrogen by employing in situ X-ray absorption and Fourier transform infrared spectroscopy. Particular focus has been directed towards the effect of oxygen on the reaction as a model system for emerging technologies for passive selective catalytic reduction of nitrogen oxides. The suppressed formation of ammonia observed as the feed becomes net-oxidizing is accompanied by a considerable increase in the oxidation state of platinum as well as the formation of surface nitrates and the loss of NH-containing surface species. In the presence of (excess) oxygen, the ammonia formation is proposed to be limited by... (More)

We study the structure-function relationship of alumina supported platinum during the formation of ammonia from nitrogen oxide and dihydrogen by employing in situ X-ray absorption and Fourier transform infrared spectroscopy. Particular focus has been directed towards the effect of oxygen on the reaction as a model system for emerging technologies for passive selective catalytic reduction of nitrogen oxides. The suppressed formation of ammonia observed as the feed becomes net-oxidizing is accompanied by a considerable increase in the oxidation state of platinum as well as the formation of surface nitrates and the loss of NH-containing surface species. In the presence of (excess) oxygen, the ammonia formation is proposed to be limited by weak interaction between nitrogen oxide and the oxidized platinum surface. This leads to a slow dissociation rate of nitrogen oxide and thus low abundance of the atomic nitrogen surface species that can react with the adsorbed hydrogen species. In this case the consumption of hydrogen through the competing water formation reaction and decomposition/oxidation of ammonia are of less importance for the net ammonia formation.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
18
issue
16
pages
6 pages
publisher
Royal Society of Chemistry
external identifiers
  • pmid:27039829
  • wos:000374786300021
  • scopus:84966277058
ISSN
1463-9076
DOI
10.1039/c5cp07624b
language
English
LU publication?
yes
id
9c8e5fc9-2640-4ab3-b4c6-1ca24835fa9a
date added to LUP
2016-09-30 07:42:41
date last changed
2024-03-07 13:07:15
@article{9c8e5fc9-2640-4ab3-b4c6-1ca24835fa9a,
  abstract     = {{<p>We study the structure-function relationship of alumina supported platinum during the formation of ammonia from nitrogen oxide and dihydrogen by employing in situ X-ray absorption and Fourier transform infrared spectroscopy. Particular focus has been directed towards the effect of oxygen on the reaction as a model system for emerging technologies for passive selective catalytic reduction of nitrogen oxides. The suppressed formation of ammonia observed as the feed becomes net-oxidizing is accompanied by a considerable increase in the oxidation state of platinum as well as the formation of surface nitrates and the loss of NH-containing surface species. In the presence of (excess) oxygen, the ammonia formation is proposed to be limited by weak interaction between nitrogen oxide and the oxidized platinum surface. This leads to a slow dissociation rate of nitrogen oxide and thus low abundance of the atomic nitrogen surface species that can react with the adsorbed hydrogen species. In this case the consumption of hydrogen through the competing water formation reaction and decomposition/oxidation of ammonia are of less importance for the net ammonia formation.</p>}},
  author       = {{Adams, Emma Catherine and Merte, Lindsay Richard and Hellman, Anders and Skoglundh, Magnus and Gustafson, Johan and Bendixen, Eva Charlotte and Gabrielsson, Pär and Bertram, Florian and Evertsson, Jonas and Zhang, Chu and Carlson, Stefan and Carlsson, Per Anders}},
  issn         = {{1463-9076}},
  language     = {{eng}},
  month        = {{04}},
  number       = {{16}},
  pages        = {{10850--10855}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Physical Chemistry Chemical Physics}},
  title        = {{The structure-function relationship for alumina supported platinum during the formation of ammonia from nitrogen oxide and hydrogen in the presence of oxygen}},
  url          = {{http://dx.doi.org/10.1039/c5cp07624b}},
  doi          = {{10.1039/c5cp07624b}},
  volume       = {{18}},
  year         = {{2016}},
}