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  Are multiple oxygen species selective in ethylene epoxidation on silver?

Carbonio, E., Rocha, T. C. R., Klyushin, A., Píš, I., Magnano, E., Nappini, S., et al. (2018). Are multiple oxygen species selective in ethylene epoxidation on silver? Chemical Science, 9(4), 990-998. doi:10.1039/C7SC04728B.

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 Creators:
Carbonio, Emilia1, 2, Author              
Rocha, Tulio C. R.3, Author
Klyushin, Alexander1, 2, Author              
Píš, Igor4, 5, Author
Magnano, Elena4, 6, Author
Nappini, Silvia4, Author
Piccinin, Simone7, Author
Knop-Gericke, Axel1, Author              
Schlögl, Robert1, 8, Author              
Jones, Travis1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II, Albert-Einstein-Straße 15, 12489 Berlin, ou_persistent22              
3Brazilian Synchrotron Light Laboratory (LNLS), Brazilian Center for Research on Energy and Materials (CNPEM), PO Box 6192, 13083-970, Campinas, SP, Brazil, ou_persistent22              
4IOM-CNR, Laboratorio TASC, S.S. 14-km 163.5, Trieste, 34149 Basovizza, Italy, ou_persistent22              
5Elettra-Sincrotrone Trieste S.C.p.A., S.S. 14-Km 163.5, Trieste, 34149 Basovizza, Italy, ou_persistent22              
6Elettra-Sincrotrone Trieste S.C.p.A., S.S. 14-Km 163.5, Trieste, Italy, ou_persistent22              
7Department of Physics, University of Johannesburg, PO Box 524, Auckland Park, 2006, Johannesburg, South Africa, ou_persistent22              
8Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion , Stiftstr. 34 - 36 45470 Mülheim an der Ruhr, Germany, ou_persistent13              

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 Abstract: The nature of the oxygen species active in ethylene epoxidation is a long-standing question. While the structure of the oxygen species that participates in total oxidation (nucleophilic oxygen) is known the atomic structure of the selective species (electrophilic oxygen) is still debated. Here, we use both in situ and UHV X-ray Photoelectron Spectroscopy (XPS) to study the interaction of oxygen with a silver surface. We show experimental evidence that the unreconstructed adsorbed atomic oxygen (Oads) often argued to be active in epoxidation has a binding energy (BE) ≤ 528 eV, showing a core-level shift to lower BE with respect to the O-reconstructions, as previously predicted by DFT. Thus, contrary to the frequent assignment, adsorbed atomic oxygen cannot account for the electrophilic oxygen species with an O 1s BE of 530–531 eV, thought to be the active species in ethylene epoxidation. Moreover, we show that Oads is present at very low O-coverages during in situ XPS measurements and that it can be obtained at slightly higher coverages in UHV at low temperature. DFT calculations support that only low coverages of Oads are stable. The highly reactive species is titrated by background gases even at low temperature in UHV conditions. Our findings suggest that at least two different species could participate in the partial oxidation of ethylene on silver.

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Language(s): eng - English
 Dates: 2017-11-012017-11-262018-01-28
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C7SC04728B
 Degree: -

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Project name : NFFA-Europe - NANOSCIENCE FOUNDRIES AND FINE ANALYSIS - EUROPE
Grant ID : 654360
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Chemical Science
  Other : Chem. Sci.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: 9 Volume / Issue: 9 (4) Sequence Number: - Start / End Page: 990 - 998 Identifier: ISSN: 2041-6520
CoNE: https://pure.mpg.de/cone/journals/resource/2041-6520