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Tracking the shape-dependent sintering of platinum-rhodium model catalysts under operando conditions.

Hejral, Uta ; Müller, Patrick ; Balmes, Olivier LU ; Pontoni, Diego and Stierle, Andreas (2016) In Nature Communications 7.
Abstract
Nanoparticle sintering during catalytic reactions is a major cause for catalyst deactivation. Understanding its atomic-scale processes and finding strategies to reduce it is of paramount scientific and economic interest. Here, we report on the composition-dependent three-dimensional restructuring of epitaxial platinum-rhodium alloy nanoparticles on alumina during carbon monoxide oxidation at 550 K and near-atmospheric pressures employing in situ high-energy grazing incidence x-ray diffraction, online mass spectrometry and a combinatorial sample design. For platinum-rich particles our results disclose a dramatic reaction-induced height increase, accompanied by a corresponding reduction of the total particle surface coverage. We find this... (More)
Nanoparticle sintering during catalytic reactions is a major cause for catalyst deactivation. Understanding its atomic-scale processes and finding strategies to reduce it is of paramount scientific and economic interest. Here, we report on the composition-dependent three-dimensional restructuring of epitaxial platinum-rhodium alloy nanoparticles on alumina during carbon monoxide oxidation at 550 K and near-atmospheric pressures employing in situ high-energy grazing incidence x-ray diffraction, online mass spectrometry and a combinatorial sample design. For platinum-rich particles our results disclose a dramatic reaction-induced height increase, accompanied by a corresponding reduction of the total particle surface coverage. We find this restructuring to be progressively reduced for particles with increasing rhodium composition. We explain our observations by a carbon monoxide oxidation promoted non-classical Ostwald ripening process during which smaller particles are destabilized by the heat of reaction. Its driving force lies in the initial particle shape which features for platinum-rich particles a kinetically stabilized, low aspect ratio. (Less)
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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
7
article number
10964
publisher
Nature Publishing Group
external identifiers
  • pmid:26957204
  • scopus:84960509989
  • wos:000371731000001
  • pmid:26957204
ISSN
2041-1723
DOI
10.1038/ncomms10964
language
English
LU publication?
yes
id
6f9cca82-88bc-4c01-a04c-080aaf59d002 (old id 8852966)
date added to LUP
2016-04-01 15:01:25
date last changed
2022-04-06 21:41:19
@article{6f9cca82-88bc-4c01-a04c-080aaf59d002,
  abstract     = {{Nanoparticle sintering during catalytic reactions is a major cause for catalyst deactivation. Understanding its atomic-scale processes and finding strategies to reduce it is of paramount scientific and economic interest. Here, we report on the composition-dependent three-dimensional restructuring of epitaxial platinum-rhodium alloy nanoparticles on alumina during carbon monoxide oxidation at 550 K and near-atmospheric pressures employing in situ high-energy grazing incidence x-ray diffraction, online mass spectrometry and a combinatorial sample design. For platinum-rich particles our results disclose a dramatic reaction-induced height increase, accompanied by a corresponding reduction of the total particle surface coverage. We find this restructuring to be progressively reduced for particles with increasing rhodium composition. We explain our observations by a carbon monoxide oxidation promoted non-classical Ostwald ripening process during which smaller particles are destabilized by the heat of reaction. Its driving force lies in the initial particle shape which features for platinum-rich particles a kinetically stabilized, low aspect ratio.}},
  author       = {{Hejral, Uta and Müller, Patrick and Balmes, Olivier and Pontoni, Diego and Stierle, Andreas}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Tracking the shape-dependent sintering of platinum-rhodium model catalysts under operando conditions.}},
  url          = {{http://dx.doi.org/10.1038/ncomms10964}},
  doi          = {{10.1038/ncomms10964}},
  volume       = {{7}},
  year         = {{2016}},
}