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

Kudernatsch, Wilhelmine; Peng, Guowen; Zeuthen, Helene; Bai, Yunhai; Merte, Lindsay R.; Lammich, Lutz; Besenbacher, Flemming; Mavrikakis, Manos; Wendt, Stefan

doi:10.1021/acsnano.5b02339

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

Journal Article · Sun May 31 00:00:00 EDT 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b02339· OSTI ID:1397273

Kudernatsch, Wilhelmine ^[1]; Peng, Guowen ^[2]; Zeuthen, Helene ^[3]; Bai, Yunhai ^[2]; Merte, Lindsay R. ^[3]; Lammich, Lutz ^[3]; Besenbacher, Flemming ^[3]; Mavrikakis, Manos ^[2]; Wendt, Stefan ^[3]

Aarhus Univ., Aarhus (Denmark); Department of Chemical and Biological Engineering, University of Wisconsin-Madison
Univ. of Wisconsin-Madison, Madison, WI (United States)
Aarhus Univ., Aarhus (Denmark)

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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Wisconsin-Madison, Madison, WI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Contributing Organization:: 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); National Energy Research Scientific Computing Center (NERSC), Pacific Northwest National Laboratory (PNNL), and Argonne National Laboratory (ANL)

Grant/Contract Number:: FG02-05ER15731

OSTI ID:: 1397273

Alternate ID(s):: OSTI ID: 1214063

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 8 Vol. 9; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO oxidation
FeO islands
Pt
active sites
catalysis
density functional theory (DFT)
in situ scanning tunneling microscopy (STM)

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

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