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          Institute: Fritz-Haber-Institut     Collection: Inorganic Chemistry     Display Documents

ID: 477787.0, Fritz-Haber-Institut / Inorganic Chemistry
Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects
Authors:Lei, Yu; Mehmood, Faisal; Lee, Sungsik; Greeley, Jeffrey P.; Lee, Byeongdu; Seifert, Sönke; Winans, Randall E.; Elam, Jeffrey W.; Meyer, Randall J.; Redfern, Paul C.; Teschner, Detre; Schlögl, Robert; Pellin, Michael J.; Curtiss, Larry C.; Vajda, S.
Date of Publication (YYYY-MM-DD):2010-04
Title of Journal:Science
Issue / Number:No. 5975
Start Page:224
End Page:228
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:Production of the industrial chemical propylene oxide is energy-intensive and environmentally unfriendly. Catalysts based on bulk silver surfaces with direct propylene epoxidation by molecular oxygen have not resolved these problems because of substantial formation of carbon dioxide. We found that unpromoted, size-selected Ag3 clusters and ~3.5-nanometer Ag nanoparticles on alumina supports can catalyze this reaction with only a negligible amount of carbon dioxide formation and with high activity at low temperatures. Density functional calculations show that, relative to extended silver surfaces, oxidized silver trimers are more active and selective for epoxidation because of the open-shell nature of their electronic structure. The results suggest that new architectures based on ultrasmall silver particles may provide highly efficient catalysts for propylene epoxidation.
Free Keywords:Silver; size effect; epoxidation
Research Context: Ag catalysts
External Publication Status:published
Document Type:Article
Communicated by:Robert Schlögl
Affiliations:Fritz-Haber-Institut/Inorganic Chemistry/Electronic Structure and Adsorption / Metals
Fritz-Haber-Institut/Inorganic Chemistry/Inorganic Chemistry
External Affiliations:Chemical Sciences and Engineering Division,
Materials Science Division,
Center for Nanoscale Materials,
X-ray Sciences Division,
Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue Argonne, Illinois 60439, USA
Department of Chemical Engineering, University of Illinois at Chicago, 810 South Clinton Street, Chicago, IL, 60607, USA
Department of Chemical Engineering, School of Engineering & Applied Science, Yale University, 9 Hillhouse Avenue, New Haven, Connecticut 06520, USA
Identifiers:URL:http://dx.doi.org/10.1126/science.1185200 [only for subscriber]
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