Selective oxidation of glycerol over carbon-supported AuPd catalysts

William C. Ketchie, Mitsuhiro Murayama, Robert J. Davis

Research output: Contribution to journalArticle

173 Citations (Scopus)

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 HAuCl4 in aqueous solution by H2. 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, H2 titration, and X-ray absorption spectroscopy at the Au LIII 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 O2, 333 K) in a semibatch reactor gave a turnover frequency (TOF) of 17 s-1 for monometallic Au and 1 s-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 H2O2 that is also formed over the Au but is detrimental to the selectivity toward glyceric acid.

Original languageEnglish
Pages (from-to)264-273
Number of pages10
JournalJournal of Catalysis
Volume250
Issue number2
DOIs
Publication statusPublished - Sep 10 2007
Externally publishedYes

Fingerprint

glycerols
Glycerol
Catalyst supports
Carbon
catalysts
Oxidation
oxidation
Catalysts
carbon
selectivity
acids
Acids
Catalyst selectivity
Polymethyl Methacrylate
Sols
X ray absorption spectroscopy
Titration
titration
Particles (particulate matter)
absorption spectroscopy

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

Selective oxidation of glycerol over carbon-supported AuPd catalysts. / Ketchie, William C.; Murayama, Mitsuhiro; Davis, Robert J.

In: Journal of Catalysis, Vol. 250, No. 2, 10.09.2007, p. 264-273.

Research output: Contribution to journalArticle

Ketchie, William C. ; Murayama, Mitsuhiro ; Davis, Robert J. / Selective oxidation of glycerol over carbon-supported AuPd catalysts. In: Journal of Catalysis. 2007 ; Vol. 250, No. 2. pp. 264-273.
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