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Title: Selective Oxidation of Glycerol over Carbon-Supported AuPd Catalysts

Abstract

Carbon-supported AuPd bimetallic nanoparticles were synthesized, characterized, and evaluated as catalysts in the aqueous-phase selective oxidation of glycerol. The bimetallic catalysts were synthesized by two different methods. The first method involved the deposition of Au onto the surface of 3-nm supported Pd particles by catalytic reduction of HAuCl{sub 4} in aqueous solution by H{sub 2}. The second method used the formation of a AuPd sol that was subsequently deposited onto a carbon support. Characterization of the catalysts using analytical transmission electron microscopy, H{sub 2} titration, and X-ray absorption spectroscopy at the Au L{sub III} and Pd K-edges confirmed that the first synthesis method successfully deposited Au onto the Pd particles. Results from the AuPd sol catalyst also revealed that Au was preferentially located on the surface. Measurement of glycerol oxidation rates (0.3 M glycerol, 0.6 M NaOH, 10 atm O{sub 2}, 333 K) in a semibatch reactor gave a turnover frequency (TOF) of 17 s{sup -1} for monometallic Au and 1 s{sup -1} for monometallic Pd, with Pd exhibiting a higher selectivity to glyceric acid. Although the activity of the bimetallic AuPd catalysts depended on the amount of Au present, none of them had a TOF greater than that ofmore » the monometallic Au catalyst. However, the AuPd catalysts had higher selectivity to glyceric acid compared with the monometallic Au. Because a physical mixture of monometallic Au and Pd catalysts also gave higher selectivity to glyceric acid, the Pd is proposed to catalyze the decomposition of the side product H{sub 2}O{sub 2} that is also formed over the Au but is detrimental to the selectivity toward glyceric acid.« less

Authors:
; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
929926
Report Number(s):
BNL-80518-2008-JA
Journal ID: ISSN 0021-9517; JCTLA5; TRN: US200822%%937
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; Journal Volume: 250; Journal Issue: 2
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; GLYCEROL; OXIDATION; CATALYTIC EFFECTS; GOLD; PALLADIUM; CATALYST SUPPORTS; CARBON; CATALYSTS; SYNTHESIS; CHEMICAL REACTION KINETICS; national synchrotron light source

Citation Formats

Ketchie,W., Murayama, M., and Davis, R. Selective Oxidation of Glycerol over Carbon-Supported AuPd Catalysts. United States: N. p., 2007. Web. doi:10.1016/j.jcat.2007.06.011.
Ketchie,W., Murayama, M., & Davis, R. Selective Oxidation of Glycerol over Carbon-Supported AuPd Catalysts. United States. doi:10.1016/j.jcat.2007.06.011.
Ketchie,W., Murayama, M., and Davis, R. Mon . "Selective Oxidation of Glycerol over Carbon-Supported AuPd Catalysts". United States. doi:10.1016/j.jcat.2007.06.011.
@article{osti_929926,
title = {Selective Oxidation of Glycerol over Carbon-Supported AuPd Catalysts},
author = {Ketchie,W. and Murayama, M. and Davis, R.},
abstractNote = {Carbon-supported AuPd bimetallic nanoparticles were synthesized, characterized, and evaluated as catalysts in the aqueous-phase selective oxidation of glycerol. The bimetallic catalysts were synthesized by two different methods. The first method involved the deposition of Au onto the surface of 3-nm supported Pd particles by catalytic reduction of HAuCl{sub 4} in aqueous solution by H{sub 2}. The second method used the formation of a AuPd sol that was subsequently deposited onto a carbon support. Characterization of the catalysts using analytical transmission electron microscopy, H{sub 2} titration, and X-ray absorption spectroscopy at the Au L{sub III} and Pd K-edges confirmed that the first synthesis method successfully deposited Au onto the Pd particles. Results from the AuPd sol catalyst also revealed that Au was preferentially located on the surface. Measurement of glycerol oxidation rates (0.3 M glycerol, 0.6 M NaOH, 10 atm O{sub 2}, 333 K) in a semibatch reactor gave a turnover frequency (TOF) of 17 s{sup -1} for monometallic Au and 1 s{sup -1} for monometallic Pd, with Pd exhibiting a higher selectivity to glyceric acid. Although the activity of the bimetallic AuPd catalysts depended on the amount of Au present, none of them had a TOF greater than that of the monometallic Au catalyst. However, the AuPd catalysts had higher selectivity to glyceric acid compared with the monometallic Au. Because a physical mixture of monometallic Au and Pd catalysts also gave higher selectivity to glyceric acid, the Pd is proposed to catalyze the decomposition of the side product H{sub 2}O{sub 2} that is also formed over the Au but is detrimental to the selectivity toward glyceric acid.},
doi = {10.1016/j.jcat.2007.06.011},
journal = {Journal of Catalysis},
number = 2,
volume = 250,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}