Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects

Journal Article · Fri Apr 09 04:00:00 EDT 2010 · Science, 328(5975):224-228

DOI:https://doi.org/10.1126/science.1185200· OSTI ID:1001484

Lei, Y; Mehmood, Faisal; Lee, Sang Soo; Greeley, Jeffrey P; Lee, Byeongdu; Seifert, Soenke; Winans, R E; Elam, J W; Meyer, R J; Redfern, Paul C; Teschner, D; Schlogl, Robert; Pellin, M J; Curtiss, Larry A; Vajda, S

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.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1001484
• Journal Information: Science, 328(5975):224-228, Journal Name: Science, 328(5975):224-228 Journal Issue: 5975 Vol. 328; ISSN SCIEAS; ISSN 1095-9203; ISSN 0036-8075
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
77 NANOSCIENCE AND NANOTECHNOLOGY
CATALYSTS
CATALYTIC EFFECTS
ELECTRONIC STRUCTURE
EPOXIDES
Environmental Molecular Sciences Laboratory
NANOSTRUCTURES
OXIDATION
PROPYLENE
SILVER