Oxidation of glycerol using gold-palladium alloy-supported nanocrystals

被引:136
|
作者
Dimitratos, Nikolaos [1 ]
Lopez-Sanchez, Jose Antonio [1 ]
Anthonykutty, Jinto Manjaly [1 ]
Brett, Gemma [1 ]
Carley, Albert F. [1 ]
Tiruvalam, Ram Chandra [2 ]
Herzing, Andrew A. [2 ]
Kiely, Christopher J. [2 ]
Knight, David W. [1 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff CF10 3AT, S Glam, Wales
[2] Lehigh Univ, Ctr Adv Mat & Nanotechnol, Bethlehem, PA 18015 USA
关键词
LIQUID-PHASE OXIDATION; SELECTIVE OXIDATION; HYDROGEN-PEROXIDE; PARTICLE-SIZE; AU; CATALYSTS; PD; H-2; NANOPARTICLES; CARBON;
D O I
10.1039/b904317a
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The use of bio-renewable resources for the generation of materials and chemicals continues to attract significant research attention. Glycerol, a by-product from biodiesel manufacture, is a highly functionalised renewable raw material, and in this paper the oxidation of glycerol in the presence of base using supported gold, palladium and gold-palladium alloys is described and discussed. Two supports, TiO2 and carbon, and two preparation methods, wet impregnation and sol-immobilisation, are compared and contrasted. For the monometallic catalysts prepared by impregnation similar activities are observed for Au and Pd, but the carbon-supported monometallic catalysts are more active than those on TiO2. Glycerate is the major product and lesser amounts of tartronate, glycolate, oxalate and formate are observed, suggesting a sequential oxidation pathway. Combining the gold and palladium as supported alloy nanocrystals leads to a significant enhancement in catalyst activity and the TiO2-supported catalysts are significantly more active for the impregnated catalysts. The use of a sol-immobilisation preparation method as compared to impregnation leads to the highest activity alloy catalysts and the origins of these activity trends are discussed.
引用
收藏
页码:4952 / 4961
页数:10
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