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Title: Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects

Abstract

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.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1001484
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Science, 328(5975):224-228
Additional Journal Information:
Journal Volume: 328; Journal Issue: 5975; Journal ID: ISSN 0036-8075
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; CATALYSTS; ELECTRONIC STRUCTURE; PROPYLENE; SILVER; CATALYTIC EFFECTS; NANOSTRUCTURES; OXIDATION; EPOXIDES; Environmental Molecular Sciences Laboratory

Citation Formats

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, and Vajda, S. Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects. United States: N. p., 2010. Web. doi:10.1126/science.1185200.
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. Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects. United States. https://doi.org/10.1126/science.1185200
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, and Vajda, S. 2010. "Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects". United States. https://doi.org/10.1126/science.1185200.
@article{osti_1001484,
title = {Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects},
author = {Lei, Y and Mehmood, Faisal and Lee, Sang Soo and Greeley, Jeffrey P and Lee, Byeongdu and Seifert, Soenke and Winans, R E and Elam, J W and Meyer, R J and Redfern, Paul C and Teschner, D and Schlogl, Robert and Pellin, M J and Curtiss, Larry A and Vajda, S},
abstractNote = {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.},
doi = {10.1126/science.1185200},
url = {https://www.osti.gov/biblio/1001484}, journal = {Science, 328(5975):224-228},
issn = {0036-8075},
number = 5975,
volume = 328,
place = {United States},
year = {Fri Apr 09 00:00:00 EDT 2010},
month = {Fri Apr 09 00:00:00 EDT 2010}
}