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Inverse single-site Fe1(OH)X/Pt(111) model catalyst for preferential oxidation of CO in H2
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.ORCID iD: 0000-0002-5459-687X
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
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2022 (English)In: Nano Reseach, ISSN 1998-0124, E-ISSN 1998-0000, Vol. 15, no 1, p. 709-715Article in journal (Refereed) Published
Abstract [en]

Inverse oxide/metal model systems are frequently used to investigate catalytic structure-function relationships at an atomic level. By means of a novel atomic layer deposition process, growth of single-site Fe1Ox on a Pt(111) single crystal surface was achieved, as confirmed by scanning tunneling microscopy (STM). The redox properties of the catalyst were characterized by synchrotron radiation based ambient pressure X-ray photoelectron spectroscopy (AP-XPS). After calcination treatment at 373 K in 1 mbar O2 the chemical state of the catalyst was determined as Fe3+. Reduction in 1 mbar H2 at 373 K demonstrates a facile reduction to Fe2+ and complete hydroxylation at significantly lower temperatures than what has been reported for iron oxide nanoparticles. At reaction conditions relevant for preferential oxidation of CO in H2 (PROX), the catalyst exhibits a Fe3+ state (ferric hydroxide) at 298 K while re-oxidation of iron oxide clusters does not occur under the same condition. CO oxidation proceeds on the single-site Fe1(OH)3 through a mechanism including the loss of hydroxyl groups in the temperature range of 373 to 473 K, but no reaction is observed on iron oxide clusters. The results highlight the high flexibility of the single iron atom catalyst in switching oxidation states, not observed for iron oxide nanoparticles under similar reaction conditions, which may indicate a higher intrinsic activity of such single interfacial sites than the conventional metal-oxide interfaces. In summary, our findings of the redox properties on inverse single-site iron oxide model catalyst may provide new insights into applied Fe-Pt catalysis. [Figure not available: see fulltext.]

Place, publisher, year, edition, pages
Springer Nature , 2022. Vol. 15, no 1, p. 709-715
Keywords [en]
atomic layer deposition, Fe1Ox/Pt(111), inverse single-site model catalyst, PROX, STM, synchrotron radiation AP-XPS, Atoms, Binary alloys, Catalysts, Interface states, Iron oxides, Metal nanoparticles, Metals, Oxidation, Reduction, Scanning tunneling microscopy, Single crystals, X ray photoelectron spectroscopy, Ambient pressures, Atomic-layer deposition, Model catalysts, Single sites, Site modeling, Synchrotron radiation ambient pressure X-ray photoelectron spectroscopy, Synchrotron radiation
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Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-311816DOI: 10.1007/s12274-021-3551-4ISI: 000664423800004Scopus ID: 2-s2.0-85115708291OAI: oai:DiVA.org:kth-311816DiVA, id: diva2:1655844
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QC 20220504

Available from: 2022-05-04 Created: 2022-05-04 Last updated: 2022-06-25Bibliographically approved

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Wang, ChunleiTissot, HeloiseWeissenrieder, Jonas

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