Digging Its Own Site

Autor(en)

Ali Rafsanjani-Abbasi, Florian Buchner, Faith J. Lewis, Lena Puntscher, Florian Kraushofer, Panukorn Sombut, Moritz Eder, Jiří Pavelec, Erik Rheinfrank, Giada Franceschi, Viktor Birschitzky, Michele Riva, Cesare Franchini, Michael Schmid, Ulrike Diebold, Matthias Meier, Georg K.H. Madsen, Gareth S. Parkinson

Abstrakt

Determining the local coordination of the active site is a prerequisite for the reliable modeling of single-atom catalysts (SACs). Obtaining such information is difficult on powder-based systems and much emphasis is placed on density functional theory computations based on idealized low-index surfaces of the support. In this work, we investigate how Pt atoms bind to the (11̅02) facet of α-Fe₂O₃; a common support material in SACs. Using a combination of scanning tunneling microscopy, X-ray photoelectron spectroscopy, and an extensive computational evolutionary search, we find that Pt atoms significantly reconfigure the support lattice to facilitate a pseudolinear coordination to surface oxygen atoms. Despite breaking three surface Fe-O bonds, this geometry is favored by 0.84 eV over the best configuration involving an unperturbed support. We suggest that the linear O-Pt-O configuration is common in reactive Pt-based SAC systems because it balances thermal stability with the ability to adsorb reactants from the gas phase. Moreover, we conclude that extensive structural searches are necessary to determine realistic active site geometries in single-atom catalysis.

Organisation(en)

Computergestützte Materialphysik

Externe Organisation(en)

Technische Universität Wien, Università di Bologna

Journal

ACS Nano

Band

18

Seiten

26920-26927

Anzahl der Seiten

8

ISSN

1936-0851

DOI

https://doi.org/10.1021/acsnano.4c08781

Publikationsdatum

10-2024

Peer-reviewed

Ja

ÖFOS 2012

103018 Materialphysik

Schlagwörter

ASJC Scopus Sachgebiete

Allgemeine Materialwissenschaften, Allgemeiner Maschinenbau, Allgemeine Physik und Astronomie

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/b71bf6cd-07d7-429d-91eb-2bc055b544f4