Selective oxidation of glycerol over carbon-supported AuPd catalysts

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

研究成果: ジャーナルへの寄稿学術誌査読

204 被引用数 (Scopus)

抄録

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.

本文言語英語
ページ(範囲)264-273
ページ数10
ジャーナルJournal of Catalysis
250
2
DOI
出版ステータス出版済み - 9月 10 2007
外部発表はい

!!!All Science Journal Classification (ASJC) codes

  • 触媒
  • 物理化学および理論化学

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