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  4. Cluster Catalysis with Lattice Oxygen: Tracing Oxygen Transport from a Magnetite (001) Support onto Small Pt Clusters
 
research article

Cluster Catalysis with Lattice Oxygen: Tracing Oxygen Transport from a Magnetite (001) Support onto Small Pt Clusters

Kaiser, Sebastian
•
Maleki, Farahnaz
•
Zhang, Ke  
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August 6, 2021
Acs Catalysis

Oxidation catalysis on reducible oxide-supported small metal clusters often involves lattice oxygen. The present work aims at differentiating whether the reaction takes place at the cluster/support interface or on the cluster. To that purpose, we trace the path of lattice oxygen from Fe3O4(001) onto small Pt clusters during the CO oxidation. While oxygen vacancies form on many other supports, magnetite maintains its surface stoichiometry upon reduction thanks to high cation mobility. To investigate whether size-dependent oxygen affinities play a role, we study two specific cluster sizes, Pt-5 and Pt-19. By separating different reaction steps in our experiment, migrating lattice oxygen can be accumulated on the clusters. Temperature-programmed desorption (TPD) and sophisticated pulsed valve experiments indicate that CO oxidation occurs with this highly reactive oxygen on the Pt clusters. Scanning tunneling microscopy (STM) shows a decrease in the apparent height of the clusters, which density functional theory (DFT) explains as a restructuring following lattice oxygen reverse spillover.

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Type
research article
DOI
10.1021/acscatal.1c01451
Web of Science ID

WOS:000684035000050

Author(s)
Kaiser, Sebastian
Maleki, Farahnaz
Zhang, Ke  
Harbich, Wolfgang  
Heiz, Ueli
Tosoni, Sergio
Lechner, Barbara A. J.
Pacchioni, Gianfranco
Esch, Friedrich
Date Issued

2021-08-06

Publisher

AMER CHEMICAL SOC

Published in
Acs Catalysis
Volume

11

Issue

15

Start page

9519

End page

9529

Subjects

Chemistry, Physical

•

Chemistry

•

size-selected clusters

•

lattice oxygen reverse spillover

•

mars van krevelen mechanism

•

magnetite

•

platinum

•

pulsed reactivity

•

stm

•

dft

•

pt-n

•

vibrational spectroscopy

•

platinum clusters

•

carbon-monoxide

•

co adsorption

•

oxidation

•

model

•

oxide

•

size

•

temperature

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LNS  
Available on Infoscience
August 28, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/180946
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