First-principles insight into CO hindered agglomeration of Rh and Pt single atoms on m-ZrO2
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
Published inCatalysis Science and Technology
© The Royal Society of Chemistry 2020
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. ...
PublisherRoyal Society of Chemistry
Publication in research information system
MetadataShow full item record
Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF; Postdoctoral Researcher, AoF
Additional information about fundingThe work was funded by Academy of Finland projects 277222 (MMK) and 307853 (MMM) and University of Jyväskylä.
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