A1 Journal article (refereed)
First-principles insight into CO hindered agglomeration of Rh and Pt single atoms on m-ZrO2 (2020)
Kauppinen, M. M., Melander, M. M., & Honkala, K. (2020). First-principles insight into CO hindered agglomeration of Rh and Pt single atoms on m-ZrO2. Catalysis Science and Technology, 10(17), 5847-5855. https://doi.org/10.1039/D0CY00413H
JYU authors or editors
Publication details
All authors or editors: Kauppinen, Minttu M.; Melander, Marko M.; Honkala, Karoliina
Journal or series: Catalysis Science and Technology
ISSN: 2044-4753
eISSN: 2044-4761
Publication year: 2020
Volume: 10
Issue number: 17
Pages range: 5847-5855
Publisher: Royal Society of Chemistry
Publication country: United Kingdom
Publication language: English
DOI: https://doi.org/10.1039/D0CY00413H
Publication open access: Openly available
Publication channel open access: Partially open access channel
Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/72100
Abstract
In this first-principles study we evaluate the thermodynamic and kinetic stability of Rh and Pt single-atoms (SAs) and subnano clusters on the monoclinic zirconia surface with and without a CO atmosphere. To address the kinetic stability and agglomeration of SAs to clusters and nanoparticles, a non-equilibrium nanothermodynamic approach is developed and parametrised using data computed with density functional theory. The bare subnano clusters are more stable than SA and become more so with increasing size, which means the agglomeration is always favoured. CO binds strongly to the single atoms and clusters, and our atomistic thermodynamics treatment indicates that some CO will be present even at ultra-high vacuum conditions. A CO atmosphere is shown to hinder cluster growth from SA, and is even capable of spontaneous cluster disintegration in the case of Pt clusters. Analysis of the CO stretching frequencies reveals that subnano clusters and single atoms should give peaks in the same region, and that using them to distinguish between surface species requires caution.
Keywords: catalysts; nanoparticles; nanostructures; noble metals; zirconium dioxide
Contributing organizations
Related projects
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Ministry reporting: Yes
Reporting Year: 2020
JUFO rating: 1