Au-Pd/AC as catalysts for alcohol oxidation: Effect of reaction parameters on catalytic activity and selectivity

被引:144
作者
Villa, Alberto [1 ]
Janjic, Nikolina [1 ]
Spontoni, Paolo [1 ]
Wang, Di [2 ]
Su, Dang Sheng [2 ]
Prati, Laura [1 ]
机构
[1] Univ Milan, Dipartimento CIMA L Malatesta, I-20133 Milan, Italy
[2] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
关键词
Gold-palladium alloy; Alcohol oxidation; LIQUID-PHASE OXIDATION; BIMETALLIC GOLD/PALLADIUM CATALYSTS; AEROBIC OXIDATION; MOLECULAR-OXYGEN; GOLD CATALYST; PALLADIUM; GLYCEROL; HYDROTALCITE; PD; MOLYBDENUM;
D O I
10.1016/j.apcata.2009.05.059
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 oxidation of different alcohols with molecular oxygen in water has been investigated using a range of activated carbon-supported Au-Pd bimetallic catalysts. The effect of the Au-Pd ratio on the conversion and selectivity was observed and a synergistic effect is present in a large range of the Au-Pd ratio, being maximized for Au-80-Pd-20 composition instead of Au-90-Pd-10 shown in glycerol oxidation [A. Villa, C. Campione, L Prati, Catal. Lett. 115 (2007) 133]. Moreover the enhancement of conversion observed by adding a base resulted greater for gold-rich catalysts rather than for palladium-rich ones. The effect of the alcohol concentration and the metal/substrate ratio in the presence or the absence of the base was also studied revealing substantial differences in terms of both activity and selectivity. At 1 M concentration under biphasic conditions benzyl alcohol has been selectively oxidized to benzalclehyde (S90 = 98%) even in the presence of NaOH with a TOF of 18,000 h(-1) using Au-60-Pd-40/AC as the catalyst. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:221 / 228
页数:8
相关论文
共 36 条
[1]   Efficient chemoselective alcohol oxidation using oxygen as oxidant.: Superior performance of gold over palladium catalysts [J].
Abad, Alberto ;
Almela, Carles ;
Corma, Avelino ;
Garcia, Hermenegildo .
TETRAHEDRON, 2006, 62 (28) :6666-6672
[2]   Selective oxidation of glycerol with oxygen using mono and bimetallic catalysts based on Au, Pd and Pt metals [J].
Bianchi, CL ;
Canton, P ;
Dimitratos, N ;
Porta, F ;
Prati, L .
CATALYSIS TODAY, 2005, 102 :203-212
[3]   Selective oxidation of glycerol to glyceric acid using a gold catalyst in aqueous sodium hydroxide [J].
Carrettin, S ;
McMorn, P ;
Johnston, P ;
Griffin, K ;
Hutchings, GJ .
CHEMICAL COMMUNICATIONS, 2002, (07) :696-697
[4]   The promotional effect of gold in catalysis by palladium-gold [J].
Chen, MS ;
Kumar, D ;
Yi, CW ;
Goodman, DW .
SCIENCE, 2005, 310 (5746) :291-293
[5]  
Choudary BM, 2001, ANGEW CHEM INT EDIT, V40, P763, DOI 10.1002/1521-3773(20010216)40:4<763::AID-ANIE7630>3.0.CO
[6]  
2-T
[7]   Solvent-free liquid phase oxidation of benzyl alcohol to benzaldehyde by molecular oxygen using non-noble transition metal containing hydrotalcite-like solid catalysts [J].
Choudhary, VR ;
Chaudhari, PA ;
Narkhede, VS .
CATALYSIS COMMUNICATIONS, 2003, 4 (04) :171-175
[8]   Supported gold nanoparticles as catalysts for organic reactions [J].
Corma, Avelino ;
Garcia, Hermenegildo .
CHEMICAL SOCIETY REVIEWS, 2008, 37 (09) :2096-2126
[9]  
DEMERIL S, 2007, APPL CATAL B-ENVIRON, V70, P637
[10]   Liquid phase oxidation of glycerol over carbon supported gold catalysts [J].
Demirel-Gülen, S ;
Lucas, M ;
Claus, P .
CATALYSIS TODAY, 2005, 102 :166-172