Ab Initio Molecular Dynamics Study of Pt Clustering on γ-Al2O3 and Sn-Modified γ-Al2O3

Simple item page
Author(s)Chen, Tso-Hsuan
Author(s)Vlachos, Dionisios G.
Author(s)Caratzoulas, Stavros
Date Accessioned2024-01-18T18:54:18Z
Date Available2024-01-18T18:54:18Z
Publication Date2023-10-05
DescriptionThis document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Physical Chemistry C, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work seehttps://doi.org/10.1021/acs.jpcc.3c04595. This article will be embargoed until 10/05/2024.
AbstractWe have conducted AIMD free energy simulations to examine the dynamics of Pt atoms and Ptn (n = 2–3) species on dry γ-Al2O3(100), dry γ-Al2O3(110), and wet γ-Al2O3(110) surfaces, with OH coverages corresponding to 500 K (11.8 OH/nm2) and 800 K (5.9 OH/nm2), while varying the Pt and Sn loading. Under the same dry conditions and temperature, comparing the (100) and (110) surface terminations revealed that the interactions between Pt and the surface play a crucial role in determining whether the potential of mean force between reduced Pt atoms is repulsive, as observed on the (100) surface, or if it can support a bound Pt–Pt state, as observed on the (110) surface. The hydration of the (110) surface had a significant impact. At a Pt loading of 0.75 Pt/nm2, with hydration of 5.9 OH/nm2, the energy of the potential of mean force increases. Although a Pt–Pt bound state is still supported, it becomes kinetically less accessible from the dispersed state. At an even higher water loading of 11.8 OH/nm2, the Pt–Pt potential of mean force becomes predominantly repulsive and can no longer sustain the Pt–Pt bound state. Higher Pt loadings of 1.12 Pt atoms/nm2 promote the aggregation of Pt into progressively larger clusters, but high levels of hydration can kinetically impede particle growth. On Sn-modified γ-Al2O3(110), Pt tends to associate with Sn, except at high levels of surface hydration where the potential of mean force between Pt and Sn atoms becomes repulsive. The presence of Sn inhibits the aggregation of Pt particles, and the Pt–Pt potential of mean force becomes increasingly repulsive with higher Sn loading.
SponsorThis work was supported by the Department of Energy’s Office of Energy Efficient and Renewable Energy’s Advanced Manufacturing Office under Award DE-EE0007888-9.5. The Delaware Energy Institute gratefully acknowledges the support and partnership of the State of Delaware toward the RAPID projects.
CitationChen, Tso-Hsuan, Dionisios G. Vlachos, and Stavros Caratzoulas. “Ab Initio Molecular Dynamics Study of Pt Clustering on γ-Al 2 O 3 and Sn-Modified γ-Al 2 O 3.” The Journal of Physical Chemistry C 127, no. 39 (October 5, 2023): 19778–87. https://doi.org/10.1021/acs.jpcc.3c04595.
ISSN1932-7455
URLhttps://udspace.udel.edu/handle/19716/33841
Languageen_US
PublisherJournal of Physical Chemistry C
Keywordscolloids
Keywordsfree energy
Keywordshydration
Keywordsnucleation
Keywordsplatinum
TitleAb Initio Molecular Dynamics Study of Pt Clustering on γ-Al2O3 and Sn-Modified γ-Al2O3
TypeArticle
Files
Original bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
Ab Initio Molecular Dynamics Study of Pt Clustering on γ-Al2O3 and Sn-Modified γ-Al2O3.pdf
Size:
6.23 MB
Format:
Adobe Portable Document Format
Description:
Main article
Download
License bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
license.txt
Size:
2.22 KB
Format:
Item-specific license agreed upon to submission
Description:
Download
Collections
Open Access Publications