Increased silver activity for direct propylene epoxidation via subnanometer size effects.
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 Ag{sub 3} clusters and {approx}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:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- DOE Contract Number:
- DE-AC02-06CH11357
- OSTI ID:
- 977369
- Report Number(s):
- ANL/MSD/JA-65945; SCEHDK; TRN: US201009%%640
- Journal Information:
- Science, Vol. 328, Issue 5975 ; Apr. 9, 2010; ISSN 0193-4511
- Country of Publication:
- United States
- Language:
- ENGLISH
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Related Subjects
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
77 NANOSCIENCE AND NANOTECHNOLOGY
99 GENERAL AND MISCELLANEOUS//MATHEMATICS, COMPUTING, AND INFORMATION SCIENCE
SILVER
CATALYTIC EFFECTS
PROPYLENE
OXIDATION
EPOXIDES
PRODUCTION
NANOSTRUCTURES
CARBON DIOXIDE
CHEMICAL REACTION YIELD
DENSITY FUNCTIONAL METHOD
CATALYSTS