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Title: Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface

Within the area of surface science, one of the “holy grails” is to directly visualize a chemical reaction at the atomic scale. Whereas this goal has been reached by high-resolution scanning tunneling microscopy (STM) in a number of cases for reactions occurring at flat surfaces, such a direct view is often inhibited for reaction occurring at steps and interfaces. Here we have studied the CO oxidation reaction at the interface between ultrathin FeO islands and a Pt(111) support by in situ STM and density functional theory (DFT) calculations. Time-lapsed STM imaging on this inverse model catalyst in O 2 and CO environments revealed catalytic activity occurring at the FeO–Pt(111) interface and directly showed that the Fe-edges host the catalytically most active sites for the CO oxidation reaction. This is an important result since previous evidence for the catalytic activity of the FeO–Pt(111) interface is essentially based on averaging techniques in conjunction with DFT calculations. As a result, the presented STM results are in accord with DFT+U calculations, in which we compare possible CO oxidation pathways on oxidized Fe-edges and O-edges. We found that the CO oxidation reaction is more favorable on the oxidized Fe-edges, both thermodynamically and kinetically.
Authors:
 [1] ;  [2] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1]
  1. Aarhus Univ., Aarhus (Denmark)
  2. Univ. of Wisconsin-Madison, Madison, WI (United States)
Publication Date:
Grant/Contract Number:
FG02-05ER15731
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 9; Journal Issue: 8; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Univ. of Wisconsin-Madison, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
National Energy Research Scientific Computing Center (NERSC), Pacific Northwest National Laboratory (PNNL), and Argonne National Laboratory (ANL); DoD High Performance Computing Modernization Program (US Air Force Research Laboratory DoD Supercomputing Resource Center (AFRL DSRC), the US Army Engineer Research and Development Center (ERDC), and the Navy DoD Supercomputing Resource Center (Navy DSRC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; active sites; catalysis; CO oxidation; density functional theory (DFT); FeO islands; in situ scanning tunneling microscopy (STM); Pt
OSTI Identifier:
1397273

Kudernatsch, Wilhelmine, Peng, Guowen, Zeuthen, Helene, Bai, Yunhai, Merte, Lindsay R., Lammich, Lutz, Besenbacher, Flemming, Mavrikakis, Manos, and Wendt, Stefan. Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface. United States: N. p., Web. doi:10.1021/acsnano.5b02339.
Kudernatsch, Wilhelmine, Peng, Guowen, Zeuthen, Helene, Bai, Yunhai, Merte, Lindsay R., Lammich, Lutz, Besenbacher, Flemming, Mavrikakis, Manos, & Wendt, Stefan. Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface. United States. doi:10.1021/acsnano.5b02339.
Kudernatsch, Wilhelmine, Peng, Guowen, Zeuthen, Helene, Bai, Yunhai, Merte, Lindsay R., Lammich, Lutz, Besenbacher, Flemming, Mavrikakis, Manos, and Wendt, Stefan. 2015. "Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface". United States. doi:10.1021/acsnano.5b02339. https://www.osti.gov/servlets/purl/1397273.
@article{osti_1397273,
title = {Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface},
author = {Kudernatsch, Wilhelmine and Peng, Guowen and Zeuthen, Helene and Bai, Yunhai and Merte, Lindsay R. and Lammich, Lutz and Besenbacher, Flemming and Mavrikakis, Manos and Wendt, Stefan},
abstractNote = {Within the area of surface science, one of the “holy grails” is to directly visualize a chemical reaction at the atomic scale. Whereas this goal has been reached by high-resolution scanning tunneling microscopy (STM) in a number of cases for reactions occurring at flat surfaces, such a direct view is often inhibited for reaction occurring at steps and interfaces. Here we have studied the CO oxidation reaction at the interface between ultrathin FeO islands and a Pt(111) support by in situ STM and density functional theory (DFT) calculations. Time-lapsed STM imaging on this inverse model catalyst in O2 and CO environments revealed catalytic activity occurring at the FeO–Pt(111) interface and directly showed that the Fe-edges host the catalytically most active sites for the CO oxidation reaction. This is an important result since previous evidence for the catalytic activity of the FeO–Pt(111) interface is essentially based on averaging techniques in conjunction with DFT calculations. As a result, the presented STM results are in accord with DFT+U calculations, in which we compare possible CO oxidation pathways on oxidized Fe-edges and O-edges. We found that the CO oxidation reaction is more favorable on the oxidized Fe-edges, both thermodynamically and kinetically.},
doi = {10.1021/acsnano.5b02339},
journal = {ACS Nano},
number = 8,
volume = 9,
place = {United States},
year = {2015},
month = {5}
}