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The Selective Species in Ethylene Epoxidation on Silver

MPG-Autoren
http://pubman.mpdl.mpg.de/cone/persons/resource/persons135780

Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons183245

Carbonio,  Emilia
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons54379

Greiner,  Mark
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons32779

Klyushin,  Alexander
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons21743

Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

http://pubman.mpdl.mpg.de/cone/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Zitation

Jones, T., Wyrwich, R., Böcklein, S., Carbonio, E., Greiner, M., Klyushin, A., et al. (2018). The Selective Species in Ethylene Epoxidation on Silver. ACS Catalysis, 8(5), 3844-3852. doi:10.1021/acscatal.8b00660.


Zitierlink: http://hdl.handle.net/21.11116/0000-0001-7352-1
Zusammenfassung
Silver’s unique ability to selectively oxidize ethylene to ethylene oxide under an oxygen atmosphere has long been known. Today it is the foundation of ethylene oxide manufacturing. Yet, the mechanism of selective epoxide production is unknown. Here we use a combination of ultrahigh vacuum and in situ experimental methods along with theory to show that the only species that has been shown to produce ethylene oxide, the so-called electrophilic oxygen appearing at 530.2 eV in the O 1s spectrum, is the oxygen in adsorbed SO4. This adsorbate is part of a 2D Ag/SO4 phase, where the nonstoichiometric surface variant, with a formally S(V+) species, facilitates selective transfer of an oxygen atom to ethylene. Our results demonstrate the significant and surprising impact of a trace impurity on a well-studied heterogeneously catalyzed reaction.