Combined in situ XPS and PTRMS Study of Ethylene Epoxidation Over Silver Full article
Journal |
Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694 |
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Output data | Year: 2006, Volume: 238, Number: 2, Pages: 260-269 Pages count : 10 DOI: 10.1016/j.jcat.2005.11.043 | ||||
Tags | Catalyst, Epoxidation, Ethylene, In situ XPS, Oxygen, PTRMS, Silver | ||||
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Abstract:
Ethylene epoxidation over silver was investigated by combined in situ X-ray photoelectron spectroscopy (XPS) and proton-transfer reaction mass spectrometry (PTRMS) at 300–520 K and 0.07–1 mbar. Ethylene oxide was present among the reaction products at T⩾420 K and p⩾0.3 mbar. The catalytically active surface contains two oxygen species – nucleophilic and electrophilic oxygen. The observed correlation between the abundance of electrophilic oxygen and the yield of ethylene oxide expressed as C2H4O partial pressure indicates that namely this oxygen species oxidizes ethylene to ethylene oxide. Opposite trend is observed for nucleophilic oxygen: the higher is the abundance of this species, the lower is the yield of ethylene oxide. This result is in line with the known fact that because of its oxidic nature, nucleophilic oxygen is active in total oxidation of ethylene to CO2 and H2O. The low activity of silver at T<420 K is caused by the presence of carbonates and carbonaceous residues at the silver surface that reduce the available silver surface area for the catalytic reaction. Reduction of the surface area available for the formation of active species due to accumulation of the embedded oxygen species also explains the decreased rate of ethylene oxide formation with time observed for T⩾470 K.
Cite:
Bukhtiyarov V.I.
, Nizovskii A.I.
, Bluhm H.
, Hävecker M.
, Kleimenov E.
, Knop-Gericke A.
, Schlögl R.
Combined in situ XPS and PTRMS Study of Ethylene Epoxidation Over Silver
Journal of Catalysis. 2006.
V.238. N2. P.260-269. DOI: 10.1016/j.jcat.2005.11.043
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Combined in situ XPS and PTRMS Study of Ethylene Epoxidation Over Silver
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Dates:
Submitted: | Mar 31, 2005 |
Accepted: | Nov 21, 2005 |
Published online: | Jan 18, 2006 |
Published print: | Mar 10, 2006 |
Identifiers:
Web of science: | WOS:000235625100003 |
Scopus: | 2-s2.0-32344440966 |
Elibrary: | 13522863 |
Chemical Abstracts: | 2006:128611 |
Chemical Abstracts (print): | 144:330972 |
OpenAlex: | W2169073867 |